Composites Part B 200 (2020) 108254

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Composites Part B
journal homepage: www.elsevier.com/locate/compositesb

Review article

Recent advancements of plant-based natural fiber–reinforced composites

and their applications☆
Mi Li a, b, Yunqiao Pu c, Valerie M. Thomas d, e, Chang Geun Yoo f, Soydan Ozcan g, h, Yulin Deng i,
Kim Nelson j, Arthur J. Ragauskas a, b, c, *
a
Department of Chemical and Biomolecular Engineering, The University of Tennessee, Knoxville, 1512 Middle Dr, Knoxville, TN, 37996, USA
b
Center for Renewable Carbon, Department of Forestry, Wildlife and Fisheries, The University of Tennessee Institution of Agriculture, 2506 Jacob Dr, Knoxville, TN,
37996, USA
c
Joint Institute for Biological Sciences, Biosciences Division, Oak Ridge National Laboratory, 1 Bethel Valley Road, Oak Ridge, TN, 37831, USA
d
School of Industrial and Systems Engineering, Georgia Institute of Technology, 755 Ferst Drive NW, Atlanta, GA, 30332-0205, USA
e
School of Public Policy, Georgia Institute of Technology, 685 Cherry Street, Atlanta, GA, 30332-0345, USA
f
Department of Paper and Bioprocess Engineering, State University of New York - College of Environmental Science and Forestry, 1 Forestry Dr, Syracuse, NY, 13210,
USA
g
Material Science and Technology Division, Oak Ridge National Laboratory, 1 Bethel Valley Road, Oak Ridge, TN, 37831, USA
h
Department of Mechanical, Aerospace, Biomedical Engineering, University of Tennessee, Knoxville, 1512 Middle Dr, Knoxville, TN, 37996, USA
i
School of Chemical and Biomolecular Engineering and RBI at Georgia Tech, Georgia Institute of Technology, North Avenue, Atlanta, GA, 30332, USA
j
GranBio LLC, 56 17th St NE, Atlanta, GA, 30309, USA

A R T I C L E I N F O A B S T R A C T

Keywords: Demands for reducing energy consumption and environmental impacts are the major driving factors for the
Polymer-matrix composites (PMCs) development of natural fiber–reinforced composites (NFRCs) in many sectors. Compared with synthesized fiber,
3D reinforcement natural fiber provides several advantages in terms of biodegradability, light weight, low price, life-cycle supe­
Mechanical properties
riority, and satisfactory mechanical properties. However, the inherent features of plant-based natural fibers have
Fiber/matrix bond
presented challenges to the development and application of NFRCs, such as variable fiber quality, limited me­
chanical properties, water absorption, low thermal stability, incompatibility with hydrophobic matrices, and
propensity to agglomeration. Substantial research has recently been conducted to address these challenges for
improved performance of NFRCs and their applications. This article reviews the recent advancements of plant-
based NFRCs, focusing on strategies and breakthroughs in enhancing the NFRCs’ performance, including fiber
modification, fiber hybridization, lignocellulosic fillers incorporation, conventional processing techniques, ad­
ditive manufacturing (3D printing), and new fiber source exploration. The sustainability of plant-based NFRCs
using life-cycle assessment and the burgeoning applications of NFRCs with emphasis on the automotive industry
are also discussed.

1. Introduction
Natural fiber–reinforced composites (NFRCs) have attracted
increasing interest as an alternative to metals and synthetic fiber­
–reinforced composites primarily because of the growing demands for
light weight in materials and a reduced environmental footprint [1].
Currently, glass fibers are the dominant reinforcing fiber in the polymer
matrix. In 2015, ~95% of the fiber composites were reinforced using
glass fibers [2]. Compared with glass fiber, natural fibers have several
advantages, such as lower density, biodegradability, abundant avail­
ability, good damping properties, less abrasive damage to equipment,
and high health safety (i.e., low skin irritation), making them a

☆
Notice: This manuscript has been authored by UT-Battelle, LLC, under contract DE-AC05-00OR22725 with the US Department of Energy (DOE). The US government
retains and the publisher, by accepting the article for publication, acknowledges that the US government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish
or reproduce the published form of this manuscript, or allow others to do so, for US government purposes. DOE will provide public access to these results of federally sponsored
research in accordance with the DOE Public Access Plan (http://energy.gov/downloads/doe-public-access-plan.
* Corresponding author. Department of Chemical and Biomolecular Engineering, The University of Tennessee, Knoxville, 1512 Middle Dr, Knoxville, TN, 37996,
USA.
E-mail address: aragausk@utk.edu (A.J. Ragauskas).

https://doi.org/10.1016/j.compositesb.2020.108254
Received 24 February 2020; Received in revised form 24 June 2020; Accepted 26 June 2020
Available online 10 August 2020
1359-8368/© 2020 Elsevier Ltd. All rights reserved.
M. Li et al. Composites Part B 200 (2020) 108254

Fig. 1. Relative comparison between natural fiber and glass fiber for composite manufacturing [6,7]. Insets are SEM photos of (left) alkaline mercerized ramie fiber
and (right) E-glass fiber.

Table 1
Typical properties of commonly studied natural fibers and several synthetic fibers.
Fiber source (or type) Density (g/cm3) Tensile strength (σ/MPa) Tensile modulus (Е/GPa) Specific modulus (Approx.) Elongation (%)

Plant-based natural fibers

Coir [14] 1.2–1.5 95–230 3–6 4 15–51
Cotton [14] 1.5–1.6 287–800 6–13 6 3–10
Flax [15] 1.53 745–1145 44–61 35 2.07
Hemp [16] 1.48 690 70 47 1.6
Jute [16] 1.3 393–773 27 21 1.5–1.8
Kenaf [14] 1.4–1.5 223–930 15–53 24 1.5–2.7
Ramie [16] 1.5 560 25 17 2.5
Sisal [14] 1.3–1.5 363–700 9–38 17 2.0–7.0
Wood pulp [17] 1.5 1000 40 27 4.4
Cellulose carbamate [18] 1.5a 365 22 15 8
Crystalline cellulose [19] 1.6 7500–7700 110–220 103 —
Cordenka rayon [18] 1.8a 833 20 11 13
Lyocell [18] 1.4a 552 23 16 11
Viscose [18] 1.3a 338 11 8 12
Synthetic fibers
Aramid [17] 1.4 3000–3150 63–67 46 3.3–3.7
Basalt [20] 2.7 2130 93 47 2
Carbon fiber (Hexcel 1.8 4330 231 129 1.8
AS4) [21]
E-glass [14] 2.5–2.6 2000–3500 70–76 29 1.8–4.8
S-glass [17] 2.5 4570 86 34 2.8

—: not reported.
a
Linear density (dtex).

promising alternative reinforcing material for composites (Fig. 1).
Additionally, life-cycle assessment (LCA) studies have reported that
NFRCs are environmentally superior to glass fiber–reinforced compos­
ites [3]. The Natural Fiber Composites Market forecast report has pro­
jected that the global NFRCs market size is expected to reach $10.89
billion by 2024, from $4.46 billion in 2016 [4]. Growing demands for
lightweight and fuel-efficient vehicles will further propel the growth of
NFRCs in the market [5].
The performance of plant-based NFRCs is determined by a synergic
combination of factors derived from the properties of reinforcing fiber,
base matrix, and the interfacial interaction of the fiber and matrix (e.g.,
mechanical interlocking, physical adhesion, chemical bonding). Despite
the great potential of natural fiber described previously, several innate
natural fiber features have been considered as major technical barriers
for the production of high-performance composites and their applica­
tions. These challenges include the heterogeneous characteristics of
natural fiber (i.e., variation in the cell wall structure, composition, and
geometry), leading to a wide variation of fiber quality; relatively lower
mechanical properties; hydrophilicity, leading to incompatibility and
aggregation tendency in hydrophobic polymer matrix; high water ab­
sorption; low thermal stability; and difficult processability into yarns
and fabrics compared with glass fibers, impeding the manufacturing of
high-performance NFRCs [8–10]. Some of these challenges of natural
fibers have been substantially addressed by recent development in, for
example, fiber treatment and modification, and process and product
innovation. The improvement in the performance of NFRCs will
continue to push forward the global demand for NFRCs and their
applications.
In this review, we provide an overview of the recent advancements of
plant-based NFRCs. Other naturally existing fibers including animal fi­
bers (i.e., protein fibers such as silk and wool) and bacterial fibers are
not covered in this review. We first briefly review the quality and me­
chanical properties of natural fibers from plants commonly used for
manufacturing NFRCs. Then, mechanical properties of NFRCs made
from three widely used thermoplastic polymer matrices—polypropylene
(PP), polyethylene (PE), and polylactic acid (PLA) are discussed, with an
emphasis on tensile properties. The strategies and breakthroughs in
improving the performance of NFRCs are then discussed and high­
lighted, including fiber treatment and modification, fiber hybridization,
incorporation of lignocellulosic fillers, advanced processing techniques,
3D printing, and exploration of new fiber resources. Finally, the life-
cycle analyses and major applications of NFRCs are briefly discussed.

2
M. Li et al. Composites Part B 200 (2020) 108254

2. Natural fibers and their mechanical properties

Lifespan (year)

Months to 100
The production of cellulose by plant photosynthesis is estimated to
be 1012 tons per year in the biosphere, making polysaccharides the

10–600

10–600

10–600
largest organic carbon reservoir [11]. The mostly studied
cellulose-based natural fibers can be categorized depending on the plant
species and plant tissue used [10,12,13], such as bast (e.g., banana, flax,
hemp, jute, kenaf, ramie, rattan), leaf (e.g., abaca, agave, banana,
cantala, coroa, curaua, henequen, istle, manila, phormium, piassava,
Surface degradation rate on land (μm/year)

pineapple, palm, sansevieria, sisal), seed and fruit (e.g., coconut, coir,
cotton, kapok, rice husk), and stalk (e.g., bagasse, bamboo, barley,
candillo, corn, isora, kudzu, nettle, oat, rape, reed, rice, rosselle, rye,
wheat, wood). Plant-based natural fibers are usually extracted from the
plant material after a retting or decortication process to remove the
undesired cell wall components (e.g., pectin, extractives, hemicellulose,
and lignin).
Several different stages are involved in manufacturing natural fibers,
including plant growth, harvesting and processing, fiber isolation, and
supplying [14]. Even from the same plant source, the properties of
20–1000
0.6–3.0
1–100

natural fiber are complicated by many factors, including physical fea­

0.5

tures, chemical composition, crystalline cellulose dimensions, microfi­

brillar angle, defects, structure, and isolation method. Consequently, the
quality and mechanical properties of the fiber can be substantially
different. Table 1 tabulates the properties of commonly studied natural
Amorphous to 90 varying on enantiomers ratio

fibers in comparison with several select synthetic fibers. The tensile

strengths and moduli of these natural fibers cover a broad span of values
with the typical tensile strength in the range of 100 to 1000 MPa. The
tensile strengths of natural fiber are generally lower than some listed
synthetic fibers (e.g., the tensile strength of E-glass fiber is about
2000–3500 MPa). This inferiority also applies to the elastic moduli of
natural fibers compared with glass fibers. However, the specific moduli
of several natural fibers (e.g., flax, hemp, kenaf, and wood pulp) are
similar or even superior to certain synthetic glass fibers when the fiber
Crystallinity (%)

density (1.2–1.6 g/cm3 for natural fiber vs. 2.5–2.6 g/cm3 for glass
fiber) is considered.
30–50

30–50

80–90

3. Mechanical properties of NFRCs

Thermoplastic and thermoset polymers have both been used as

matrices for natural fibers. Because most natural fibers are not thermally
stable above 200 ◦ C, thermoplastics that soften and thermosets that can
Density (~23 ◦ C)

be cured below this temperature are in turn selected as a matrix [22].

Due to the easy recycling potential of thermoplastics, four types of
0.91–0.93

0.96–0.97

1.21–1.25

matrices (i.e., PP, low-density PE [LDPE], high-density PE [HDPE], and

0.90

PLA) have been widely used for NFRCs. The major chain structure,
Selected features of major commercial thermoplastic polymers [23–25].

physical features, and degradability of the four matrices are compared

in Table 2. The mechanical properties of their fiber–reinforced com­
posites are discussed separately in the following sections.
Tg (◦ C)

55–65
~100

3.1. Natural fiber–reinforced PP

~25

~80

PP is widely used as a matrix for NFRCs because of its processing

suitability (i.e., filling, reinforcing, and blending), affordability, low
heat distortion temperature, transparency, flame resistance, and
dimensional stability [26]. Although the tensile properties of natural
fiber/PP composites exhibit a wide distribution, incorporating natural
Chain structure

fibers can substantially increase the elastic modulus and the tensile
strength of the matrix depending on the fiber content and incorporation
methods (Fig. 2). Compared with the tensile properties of 20 wt % long
glass fiber–reinforced PP (orange dotted line in Fig. 2) that is specified
for interior applications from Ford Motor Company [27], many NFRCs
with fiber content higher than 30 wt % have attained higher tensile
modulus values. However, the tensile strengths of NFRCs are typically
lower than this glass fiber/PP composite, which is historically attributed
Polymer
Table 2

HDPE
LDPE

to the incompatibility between natural fiber and the matrix. This lower
PLA
PP

tensile strength could be also associated with the low transverse

3
M. Li et al.
mechanical properties of natural fiber relative to glass fiber.
Interestingly, bamboo fiber has shown higher physical and chemical
compatibility with PP than glass fiber as revealed by the better combi­
nation of wetting parameters (e.g., higher work of adhesion, higher
spreading coefficient, higher wetting tension, and lower interfacial en­
ergy) [28]. However, the glass fiber exhibited higher interfacial bonding
strength in the composites, indicated by both higher critical local
interfacial shear stress value and radial normal stress at the moment of
crack initiation, which explained that the overall performance of
bamboo fiber was weaker than glass fiber in reinforcing PP. This result
supports the idea that the anisotropic nature of natural fibers is likely the
primary reason for its lower interfacial properties and stress transfer
capability at the fiber/matrix interface compared with glass fiber.
Thomason reported that the transverse and shear modulus of jute fiber is
an order of magnitude lower than the longitudinal modulus [29].
Therefore, the general lower mechanical performance of NFRC to the
glass fiber–reinforced composites analog is primarily attributed to the
low mechanical properties in the transverse direction with the potential
detachment of the outer layer and elementary fibers in contact with the
matrix, often the case in compounding and extrusion, rather than the
physical and chemical compatibility between the fiber and matrix.
3.2. Natural fiber–reinforced PE
PE is generally divided into LDPE and HDPE based on its density and
branching. LDPE has relatively long branches with a random packing
pattern and low crystallinity, whereas HDPE consists of long chains
(without major branching) with a regular packing pattern and high
crystallinity [31]. Similar to natural fiber/PP composites, the tensile
properties of natural fiber/PE composites exhibited a wide distribution,
but the tensile strength and elastic modulus can be both substantially
reinforced by natural fibers (Fig. 3). Compared with the 20 wt % glass
fiber–reinforced HDPE (orange dotted line in Fig. 3) [32], higher stiff­
ness and comparable tensile strength of NFRCs can be achieved. In
particular, the NFRC composites fabricated from natural fibers in mat or
stacking sheets demonstrated promising potential as an alternative to
glass fiber–reinforced composites [33]. For example, the HDPE com­
posite with 40 wt % kenaf fiber mat showed a specific tensile strength of
50 MPa cm3/g, tensile modulus of 6.3 GPa cm3/g, flexural strength of
72.9 MPa cm3/g, and flexural modulus of 3.9 GPa cm3/g, which are
comparable to the 40 wt % discontinuous glass fiber/HDPE counterpart
with 47 MPa cm3/g, 6.6 GPa cm3/g, 66.1 MPa cm3/g, and 4.4 GPa
cm3/g, respectively. A similar process combining an adhesive coating of
flax fabric, sandwiching coated fabric with polymer films, and
compression molding of multilayer prepregs obtained flax/PE composite
with exceptionally impressive tensile strength of 180–280 MPa and
tensile modulus of 15–22 GPa [34].
3.3. Natural fiber–reinforced PLA
PLA has emerged as an interesting matrix with outstanding physical
and mechanical properties, renewability, and biodegradability. Addi­
tionally, PLA has special qualities including good transparency and
processability, glossy appearance, and high rigidity for NFRC
manufacturing, although it has some shortcomings such as low thermal
stability, brittleness, and high rate of crystallization [36]. Compared
with the 20 wt % glass fiber–reinforced PLA [37], many NFRCs have
achieved higher tensile strengths and moduli (Fig. 4). The mechanical
properties of PLA composites can be significantly enhanced by con­
trolling the fiber content, fiber length [38], fiber direction [39], prepreg
4
Composites Part B 200 (2020) 108254
form [40], and woven structure [41]. For example, the composite made
from wood pulp sheets compressed with PLA film attained significantly
improved tensile properties (σ of 121 MPa and E of 10.5 GPa) to the neat
PLA (σ of 60 MPa and E of 3.5 GPa) [40]. This wet-laid paper-making
method showed several advantages including uniform dispersion of
fiber, minimal reduction of fiber aspect ratio and mechanical damage,
and high fiber fraction.
The tensile properties of PLA composites can also be significantly
improved when incorporating unidirectional natural fibers. For
example, PLA with 44 vol % unidirectional flax had a specific tensile
strength of 252.3 MPa cm3/g and modulus of 14.9 GPa cm3/g in the fiber
direction that were even slightly superior to the 43–50 vol % woven
glass fiber–reinforced epoxy [39]. The unidirectional nature of natural
fiber maintained great reinforcement in the composite strength and
modulus that were even better than PLA composites made with fibers in
mat layers and injection molded short fiber composites. The measured
fiber orientation factor of PLA composites made from aligned discon­
tinuous harakeke and hemp fiber showed higher values than the com­
posites prepared using injection and compression with randomly
oriented fiber mats, but slightly lower than those obtained with aligned
fiber nonwoven preform composites [42]. When fibers are aligned
parallel to the loading direction with high interfacial bonding, the stress
transfer from the matrix to fiber becomes more effective, thus leading
the composite to a larger strength and stiffness. However, too much fiber
content in the mat can reduce fiber orientation factor due to a higher
degree of fiber agglomeration. Additionally, compared with glass fiber,
natural fiber also tends to bend and twist in the matrix during extrusion
and molding process, which could adversely influence the toughness and
strengths of composites [43].
Although certain NFRCs have achieved performance comparable to
glass fiber–reinforced composites [33,34,39], NFRCs still exhibit several
detrimental problems that have impeded their widespread applications.
The challenges associated with NFRCs include (1) wide distribution of
mechanical performance due to the heterogeneous physicochemical
nature of natural fiber, various fiber isolation, and composite fabrication
methods; (2) relatively low mechanical properties and durability
restricting NFRC applications to nonstructural and interior components;
(3) incompatibility of hydrophilic fiber with primarily hydrophobic
matrices; (4) high water absorption of natural fiber causing comprised
mechanical properties; (5) difficult dispersion of natural fiber in poly­
mer matrix due to aggregation tendency and physical entanglement; and
(6) low thermal stability resulting in restriction in the temperature range
of manufacturing, processing, and final applications.
4. Strategies for enhancing the performance of NFRCs
Most NFRCs using the three common polymer matrices have
maximum tensile strengths and moduli in the range of 20–140 MPa and
1–10 GPa (Figs. 2–4), respectively, which are low for primary and load-
bearing components. This lower mechanical performance of NFRCs
derives from several factors associated with NFRCs, such as heteroge­
neous characteristics of natural fiber leading to a wide variation of fiber
quality; hydrophilicity leading to incompatibility and aggregation ten­
dency in hydrophobic polymer matrix, high water absorption, low
thermal stability; and difficult processability into yarns and fabrics
compared with glass fibers. Several strategies, such as fiber treatment
and modification, hybridization and structural configuration, incorpo­
ration of nanocellulose, manufacturing process advancement, 3D
printing, and new plant fiber exploration have been used to negate these
disadvantages.
M. Li et al. Composites Part B 200 (2020) 108254

Fig. 2. Comparison of the reported tensile strengths (σ ) and moduli (E) of natural fiber–reinforced PP. Volume fiber fraction is used if the weight loading fraction is
not reported. The black dotted line represents the properties of neat PP (σ of 28 MPa and E of 0.69 GPa) [30] and the orange dotted line represents the properties of
20 wt % long glass fiber (GF)–reinforced PP specified for interior applications from Ford Motor Company (σ of 64 MPa and E of 4.1 GPa) [27]. The complete numbers
with each reference are included in the supplementary file. (For interpretation of the references to colour in this figure legend, the reader is referred to the Web
version of this article.)

Fig. 3. Comparison of the reported tensile strengths (σ) and moduli (E) of natural fiber–reinforced PE. Volume fiber fraction is used if the weight loading fraction is
not reported. The black dotted line represents the properties of a neat HDPE (σ of 19.6 MPa and E of 0.74 GPa) [35] and the orange dotted line represents the
properties of 20 wt % glass fiber (GF)–reinforced HDPE (σ of 42 MPa and E of 1.4 GPa) [32]. The complete numbers with each reference are included in the
supplementary file. (For interpretation of the references to colour in this figure legend, the reader is referred to the Web version of this article.)

4.1. Fiber treatment and modification
The incompatibility and poor adhesion of natural fiber in a polymer
matrix are usually addressed by fiber treatment and modification to
enhance effective wetting and uniform dispersion (Fig. 5). The primary
techniques used for fiber treatment and modification can be grouped
into fiber pretreatment (e.g., mercerization), surface coating modified
with coupling agents, and in situ compatibilization during processing
depending on the practical applications. Mercerization, a chemical
treatment using alkali, is widely used to fibrillate and purify fibers
(partially removing oil, wax, pectin, hemicellulose, and lignin) prior to
composite fabrication [45–48]. Fiber treatment with alkali has shown at
least four favorable effects to the mechanical properties improvement of
NFRCs: (1) increased cellulose content and the degree of crystallinity,
which is indicative of higher fiber strength and stiffness; (2) increased
surface roughness topography for better mechanical interlocking be­
tween the fiber and matrix; (3) increased cellulose exposure for
increased bonding/reaction sites on the fiber surface; and (4) increased
surface energy for better wetting and compatibility. Treatment with a
mild alkaline condition (~5 wt %) is typically sufficient to remove fiber
impurities with minimal impact on the fiber texture and structure
whereas higher alkaline concentration can lead to excessive removal of
lignin and fiber damage [46,49–52].
Incorporating a coupling agent (e.g., maleic anhydride [MA]–grafted
copolymer and silane agent) is another approach to improve the overall
quality of NFRCs by enhancing interfacial bonding [55–58]. The anhy­
dride groups of the MA-grafted copolymers can esterify with the surface
hydroxyl groups of natural fiber and reduce hydrogen bond formation.

5
M. Li et al.
Fig. 4. Comparison of the reported tensile strengths (σ) and moduli (E) of natural fiber–reinforced PLA. Volume fiber fraction is used if the weight loading fraction is
not reported. The black dotted line represents the properties of neat PLA (σ of 54.36 MPa and E of 3.23 GPa) [37] and the orange dotted line represents the properties
of 20 wt % glass fiber (GF)–reinforced PLA (σ of 67.9 MPa and E of 6.7 GPa) [44]. The complete numbers with each reference are included in the supplementary file.
(For interpretation of the references to colour in this figure legend, the reader is referred to the Web version of this article.)
The other part of the copolymer with similar polarity entangles with the
polymer matrix for improved compatibility. A recent study showed that
the coupling agent not only affected the nucleation process but also
increased crystallization kinetics [59]. The isothermal crystallization
studies of the composites revealed different crystallization kinetics of
miscanthus/PP with and without the addition of MA-grafted PP (MAPP)
in that the crystallization started earlier with larger values of the kinetic
constant for the NFRCs containing MAPP. The study also suggested that
the fiber size affects the crystallization process of the composite only
when the MAPP is added—the rate constant of the PP crystallization
increases gradually as the size of the miscanthus stem fragments is
reduced. The increased surface area associated with fiber size reduction
is linked with the increased nucleating capacity of fiber fragments acting
as a nucleating agent. For non-coupled composites, the size of fiber
fragments did not significantly influence the crystallization kinetics of
miscanthus/PP. MA-grafted PLA is not as readily available as MAPP.
However, its addition has shown improved interfacial adhesion for
kenaf, wheat straw, coconut fiber, ramie, wood fiber, and reishi
(Ganoderma lucidum) fiber in PLA composites [60–62].
El-Sabbagh performed a systematic work of different parameters,
including coupling agent weight ratio to the fiber, coupling agent
source, fiber type, and fiber weight content, to optimize the MAPP
amount in natural fiber/PP composites [63]. The optimal stiffness,
tensile, and impact strengths varied depending on the coupling agent
loading as well as the fiber type, fiber loading, and coupling agent
source. The MAPP to fiber ratio required for maximizing stiffness was
less than that needed for tensile and impact strength. Taken together,
6.7 wt % of the coupling agent to fiber was found sufficient for signifi­
cant improvement in mechanical properties. However, excessive MAPP
did not increase the coupling effect with fibers but instead led to
self-reaction and weak layers. Additionally, the interfacial adhesion and
mechanical and thermal stability of the MAPP-coupled composites
strongly depended on the amount of MA-grafting level and the MAPP
molecular weight [64]: (1) a low MA-grafting level did not offer suffi­
cient interaction with natural fiber whereas an excessively high MA
percentage may restrict the interaction of MAPP with the matrix; and (2)
MAPP with low molecular weight entangled insufficiently with the
matrix whereas excessively high molecular weights of MAPP restricted
6
Composites Part B 200 (2020) 108254
its residence at the MAPP/matrix interface.
Silane coupling agents are another “family” of compounds
commonly applied to fibers to increase the interfacial bonding of the
fiber and matrix [53,65]. The chemical modification of fibers with a
silane agent undergoes the following major steps [65]: (1) hydrolysis of
the silane agent to liberate reactive silanol group in the presence of
water; (2) self-condensation of silanols (this step should be minimized
usually by controlling pH); (3) physical absorption of reactive silanol
compound to hydroxyl groups of the fiber through hydrogen bonding;
and (4) grafting to form covalent –Si–O–C– bonds between silanol and
hydroxyl groups upon heating. The functions of different silane treat­
ment parameters, such as the concentration of the organosilane solution,
soaking time, and treatment temperature, have been studied on flax/­
PLA composites. Flax fiber treated with 5–10 wt % (3-glycidylox­
ypropyl) trimethoxysilane at 70 ◦ C was recommended for the optimum
organosilane treatment conditions, resulting in 20–25% higher yield
stress than the composite without fiber treatment [66]. Treatment with
γ-methacryloxypropyltrimethoxysilane had greater efficiency in hemp
fiber fragmentation and a greater improvement in the tensile modulus of
the PP/hemp composites than the other two silane agents, (γ-amino­
propyltriethoxysilane, γ-glycidoxypropyltrimethoxysilane) [67]. The
superior treating effect of γ-methacryloxypropyltrimethoxysilane was
attributed to more stable adsorption and interaction to hemp fiber and
less lubricating and self-condensation.
Fiber/matrix adhesion has been advanced through interfacial to­
pology analysis of single-fiber composites. The interfacial shear strength
of single sisal fiber/PP composite was found to be closely correlated with
three types of crystalline interfacial crystalline morphologies: spheru­
lite, medium–nuclei density transcrystallinity (MD-TC) and high–nuclei
density transcrystallinity (HD-TC) (Fig. 6) [68]. The transcrystalline
superstructure depicts a columnar crystalline layer covering the fiber
surface, and its growth varies on the nucleus density on the surface of the
fiber. At low nucleus density, the crystals grew in both parallel and
perpendicular directions to the fiber axis, namely MD-TC; at high nu­
cleus density due to the presence of MAPP and shear-induced pulling,
the crystal grew perpendicularly to the fiber axis, namely HD-TC.
Compared with the amorphous conditions, the transcrystalline super­
structure showed significantly higher interfacial shear strength, 95% for
M. Li et al.
Fig. 5. Examples of typically reported methods for treating and modifying natural fibers [53,54].
MD-TC and 178% for HD-TC. This increase was attributed to the inter­
phase thermal shrinkage, leading to a high contraction force that can
distribute the stress down to the atomic scale to affect the mechanical
interlocking.
To promote the epitaxial growth of this transcrystalline structure, the
addition of a rare earth compound into sisal/PP and cotton/PP systems
triggered the rare earth compound adsorption onto the surface of natural
fiber due to hydrogen bonding between the amide groups of the rare
earth compound and the hydroxyl groups of fiber [69,70]. The intro­
duced particle generated a root-like fiber with an interfacial interlocking
effect that significantly increased the interfacial adhesion, leading to
higher interfacial shear strength, interfacial friction, and debonding
energy [69]. Similarly, in another study, coating with few-layer gra­
phene oxide nanosheets to ramie fiber showed significantly increased
shear strengths in PLA [71]. Coverage of graphene nanosheets on ramie
through hydrogen bonding exhibited a prominent capability to trigger
the generation of highly ordered transcrystallinity of PLA composite
with a higher orientation degree. These findings suggest that manipu­
lating the formation of transcrystalline structures accompanied by
enhanced interfacial shear strength may be an effective method for
improving the mechanical properties of NFRCs. However, a more recent
study has shown that coating wood fiber in PP with nucleating agents
modified the matrix crystallinity and the transcrystallinity of the fiber
and matrix, but had little influence on the mechanical properties com­
posites [72]. This suggests the addition of nucleating agents likely has
little influence on interfacial adhesion.
4.2. Fiber hybridization
Fiber hybridization has been attempted to balance the deficiency of
one specific fiber to achieve sustainability, low cost, and improved
performance of NFRCs [73,74]. Hybridization methods provide flexi­
bility in fibers selection for engineering materials properties according
to the application requirements. Fiber hybrid composites are typically
produced by hybridizing natural fibers with another either natural or
synthetic fiber(s) with superior properties, such as mechanical strength,
chemical stability, nontoxicity, noncombustible, resistance to high
temperatures, and thermal or acoustic insulation. Fiber hybridization is
usually accomplished either via intermingling of different types of fibers
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Composites Part B 200 (2020) 108254
as a mixture or interlaminating layers of different fibers before their
addition to the matrix [75].
Hybridization of natural fibers with synthetic fibers, such as glass,
carbon, Kevlar, basalt fibers, and carbon nanotubes, can significantly
enhance the mechanical performance of NFRCs. For example, the hy­
bridization of jute fabric with glass fiber fabric (1:1 wt ratio) has
improved the tensile and impact strengths jute fabric–reinforced poly­
ester by three-fold and six-fold, respectively; similarly, almost ten-fold of
tensile strength and five-fold of the impact strength improvement are
obtained by hybridizing jute fabric with carbon fibers [76]. To reduce
the composite discrepancies due to shrinkage and warpage, the flow and
cross-flow shrinkage values of the sisal/glass fiber/PP hybrid composite
can be optimized by controlling the injection molding process parame­
ters, thus meeting the material’s maximum shrinkage requirements for
under-the-hood parts used in the automotive industry [77]. Hybrid
composites of natural fiber with other natural fibers may not show
comparable mechanical improvements to those hybridized with syn­
thetic fibers, but this approach may have significant value in terms of
sustainability. For example, a mixture of pineapple leaf fiber and fibers
extracted from recycled bamboo chopsticks at 30 wt % improved the
tensile strength, modulus, flexural strength, and modulus of neat PLA by
66.1%, 216%, 66%, and 121%, respectively [78]. This hybridization
with PLA and poly(butylene succinate) can lead to fully biodegradable
composites.
The ultimate performance of the hybrid composite is determined by
several factors, such as fiber content, hybrid ratio, fiber orientation [79,
80], stacking sequences [76,81–83], and innate fiber features. The
tensile strength and failure strain of the hybrid composite increased
from ~200 MPa to 0.9% for flax-alone reinforced composites to ~700
MPa and 1.4% for glass fiber–alone reinforced composites [84]. With a
higher glass fiber hybrid volume fraction, the hybrid composite main­
tained its integrity until the failure dominated by the bigger failure
elongation of glass fiber. Interestingly, the hybrid composite had a
higher interlaminar shear strength compared with the composites
reinforced with either natural or glass fiber alone. This was explained by
an increase in interlaminar fracture toughness from the twisted flax yarn
structures and rough surface that led to the bridging and entangling of
interfaces.
Hybridization can compensate for the inherent disadvantages of the
M. Li et al.
Fig. 6. Micrographs revealing transcrystalline structure in a sisal fiber/PP composite. (a and b) Polarized optical images and (c and d) SEM images show three types
of crystalline structures: spherulite (arrows in a and b), MD-TC (a and c), and HD-TC (b and d). Picture adapted from Ref. [68] with permission from Wiley.
individual bioresources. For example, Yusoff et al. observed that the
different stacking configurations of the hybrid PLA composite with kenaf
(K)/bamboo(B)/coir(C) showed a diverse range of mechanical proper­
ties results [85]. With the same total fiber content (60 wt %), the
stacking sequence of KBCCBK increased the neat resin tensile strength
from 25 to 187 MPa and the modulus from 1.7 to 7.5 GPa. The increased
tensile strength was about 20 and 78% higher than composite sequences
of KCCK and BCCB, whereas the modulus was only 2 and 25% higher
than those of KCCK and BCCB, respectively. The high Young’s modulus
of kenaf and bamboo fibers contributed better in resisting loads at the
outer layers of composites, while the high ductile coir fiber offset the low
elongation of the kenaf and bamboo fibers in the composites. In terms of
the flexural properties, the PLA/BCCB and PLA/KBCCBK composites had
about 20% higher flexural strength but 70% lower flexural modulus than
the PLA/KCCK composite. This higher flexural modulus of the
PLA/KCCK composite was explained by the lumen connected to the
secondary layer of the kenaf and coir fibers, which promoted cohesion
by interlocking the fiber cell walls with the PLA matrix. The results
suggest that high-strength and -modulus fibers in the outer layers and
effective matrix impregnation into lumen are key factors for hybridi­
zation configuration maintaining superior mechanical performance. A
recent study of the fiber aspect ratios in kenaf/corn husk for hybrid
composites pointed out that hybrid fillers with similar dimensions (i.e.,
the aspect ratios of the reinforcing fibers are close to each other) were
effective in external force transfer and modulus enhancement, which
could be an indicator in optimizing the mechanical properties of a
hybrid composite [86]. Also, Kwon et al. found that the aspect ratio of
8
Composites Part B 200 (2020) 108254
fibers before the extrusion process can be used directly to predict the
mechanical properties because the aspect ratio after extrusion does not
show a significant difference in the tensile modulus calculation.
4.3. Incorporation of nanocellulosic fillers
Recently, lignocellulosic nanofillers, such as cellulose nanocrystals
(CNCs) and cellulose nanofibrils (CNFs), have emerged as attractive
reinforcing materials due to their substantial specific surface areas, high
crystal stiffness, strength, and maintained aspect ratio [87–89]. Crys­
talline cellulose was reported to have a tensile strength of 7.5 GPa and
modulus of 110–220 GPa [19]. Similar to inorganic fillers, the micro-
and nano-scaled fillers provide a large surface for linking and bonding
the matrix, which is beneficial for physical adhesion at the interface,
stress transfer, and ultimate mechanical properties of the composite
[90]. Table 3 lists select CNC– and CNF–reinforced composites and their
essential properties. However, incompatibility and aggregation of
nanocellulose in matrix remain the top challenges for fabricating
high-performance nanocellulose composites.
With nanometric fillers, superior mechanical, thermal, and barrier
properties can be achieved at low reinforcement concentration, usually
<10 wt %. For example, softwood CNF–reinforced epoxy resin showed
maximum values of tensile strength and modulus, impact strength,
flexural strength and modulus, and elongation at 0.75 wt % fiber loading
[97]. Reinforcement with a high concentration of nanocellulose fillers
adversely leads to several problems, such as aggregation of nanofibers,
reduction in fiber/matrix interfacial adhesion, restricted consolidation
M. Li et al. Composites Part B 200 (2020) 108254

Table 3
Nanocellulose fiber–reinforced composites and their major properties.
Nanocellulose Polymer matrix Tensile strength (MPa) E (GPa) Other key changes Ref.

CNC (Kraft pulp) LDPE — 0.16 → 0.27 ↓ Thermal degradation [91]

↑ Creep performance
CNC (Kraft pulp) PP — 1.2 → 1.8 ↓ Strain, thermal degradation [91]
↑ Creep performance
CNC (bleached jute) Epoxy 44 → 40 4.6 → 5.6 ↑ Flexural strength and modulus, fracture toughness, E′ [92]
↓ Tg, damping factor
CNC (bleached kenaf) Polyester 40 → 48 0.8 → 0.9 ↑ Impact energy, Tg, E′ [93]
CNC (bleached agave, 1%) PLA 45 → 37 2.7 → 3.5 ↓ Tc [94]
CNF (eucalyptus Kraft pulp) Epoxy 11 → 14 15% higher ↑ Tribological behavior [95,96]
↓ Tg
CNF (bleached agave, 2%) PLA 45 → 35 2.7 → 3.0 ↓ Tc [94]
CNF (bleached softwood) Epoxy 21 → 27 0.6 → 1.3 ↑ Strain, impact strength, flexural strength and modulus [97]
CNF (bleached softwood) HDPE 22 → 43 1.1 → 2.0 ↓ Strain [98]
CNF (bleached carrot) Cellulose acetate butyrate — 2.1 → 3.5 ↑ E′ [99]
Microfibrillated cellulose PP 28 → 26 1.9 → 3.1 ↑ Flexural strength and modulus [100]
↓ Viscosity

E: Young’s modulus; —: not reported; E’: storage modulus Tg: glass transition temperature; Tc: crystallization temperature; → shows the improvement from the neat
polymer to the reinforced composite.

of composites during the crosslinking process, defects generation in the
composites, ineffective stress transfer, and ultimately, compromised
composite performance. Surface treatment of nanocellulose (e.g., silane
agent, alkenyl succinic anhydride) is an applicable method to moderate
nanofiber agglomeration and improve interfacial adhesion [93,94,98].
In theory, a well-dispersed mixture of 40 wt % CNF in cellulose acetate
butyrate could increase the tensile modulus of the matrix from 2.07 GPa
to 11 GPa [99]. The aspect ratio of nanocellulose is also critical for the
high performance of nanocellulose–reinforced composites. By
comparing the reinforcing effects of CNCs with different sizes isolated
from the same biomass, high–aspect ratio CNCs were recommended not
only because they decrease the percolation threshold and reinforcing
capability at low CNC content, but also because the upper modulus limit
corresponding to high CNC content was higher [101].
Another study of nanocomposites comparing CNF– and CNC–rein­
forced polyurethane revealed that CNFs with higher aspect ratio had
better mechanical and thermal property improvement than CNCs [102].
Benhamou et al. also found that the residue of hemicellulose and lignin
in CNFs resulted in better interfacial compatibility with the polymer.
Similarly, Graupner et al. showed that lignin doping was beneficial for
bonding and apparent interfacial shear strength of Lyocell fiber in PLA,
MAPP, and PP matrices [103]. These benefits were generally attributed
to several factors, including (1) the addition of lignin reduced the vis­
cosity of PLA matrix; (2) exfoliated lignin particles led to a higher spe­
cific fiber surface for interfacial bonding; and (3) chemical interactions
were improved between the fiber and matrix via the van der Waals force.
4.4. Advancement of conventional manufacturing processes
Extrusion, injection molding, compression molding, sheet stacking,
and resin transfer molding are the most commonly used methods for
manufacturing NFRCs. Process parameters such as compounding time,
molding temperature, pressure, and compression time remain a complex
balance but have a significant impact on the mechanical properties of
NFRCs, such as wood flour/PP [104], flax/PLA [105], bamboo/epoxy
[106], and kenaf/HDPE [107]. Studies have suggested that (1) wetting
and homogeneous dispersion of fibers are the most crucial targets during
NFRCs processing; (2) a relatively higher processing temperature and
pressure generally have a better impact on rheological properties and
penetration of polymer into the natural fibers, whereas the press/hold
time has only a small impact; and (3) the thermo-chemical degradation
of natural fibers should be considered as the maximum consolidation
time to avoid major degradation of the composite mechanical strength.
To reduce fiber attrition during processing, a direct-injection molding
process (i.e., sisal and PLA pellets were directly fed into an
injection-molding machine) showed significantly superior capability in
maintaining fiber lengths compared with the extrusion-injection sepa­
rate molding process [108]. However, the composites made from
direct-injection molding had lower tensile and flexural properties than
those of extrusion-injection molding, which was attributed to the for­
mation of fiber clusters hindering adequate wetting of the fibers and
acting as stress concentration under mechanical testing.
The effective dispersion of fibers is crucial for manufacturing high-
performance NFRCs. A study of twin-screw extrusion of Cordenka cel­
lulose/polyamide found that the extrusion temperatures and screw
configurations caused only minor effects on the morphological structure
and the mechanical properties of the composite and much more influ­
ence on fiber length distribution and dispersion [109]. Another study of
kenaf/PP composites also noted that an effective fiber dispersion after
the extrusion-injection process resulted in significantly improved me­
chanical performance irrespective of the initial fiber length [110]. The
twin-screw extrusion of jute/PLA with a combined configuration that
reduced the compounding shear stress and enhanced the distributive
mixing greatly improved the overall fiber dispersion. This compounding
process facilitated the dispersion of the jute yarn to bundle and the
de-cohesion of the bundle to elementary fibers, leading to efficient
strength transfer from matrix to fiber [111]. Short fiber–reinforcement
was found to exhibit better PLA coating on the pullout fibers of the
fractured composite compared with the long jute fiber–reinforcement
(higher aspect ratio) (Fig. 7). A recent study of injection-molded
hemp/PP composites discovered that fiber content increased along the
spiral flow length (i.e., longer fibers usually at the end of the injected
part and shorter fibers near mold entrance point) [112]. The fiber con­
tent reached up to 30% deviation at different molding conditions, sug­
gesting that the homogeneity of fiber weight content along the injection
mold spiral acted as an essential quality feature [113]. Usually, a
solid-state shear pulverization process is used to facilitate the dispersion
and orientation of the filler particles within the polymeric matrix [91,
114].
Recently, a new twin-screw processing method was developed that
enables continuous micro-fibrillation of pulp and its melt compounding
with PP [115]. In this method, never-dried pulp and PP powder were

9
M. Li et al. Composites Part B 200 (2020) 108254

Fig. 7. SEM micrographs of the fracture surface of composites reinforced with (a) long fiber pellets and (b) short fiber pellets. Reproduced from Ref. [111] with
permission from Elsevier.

kneaded via a twin-screw extruder. During the melt compounding pro­
cess, the water content was minimized by evaporation and the pulp was
defibrillated and entangled in the powdered PP rather than the forma­
tion of microfibril cellulose aggregation. With the addition of 6.7 wt %
MAPP, the PP composite with 50 wt % Kraft pulp had twice the tensile
strength and 1.5 times the modulus of neat PP. The mechanical prop­
erties of PP composites were further improved when a cationic polymer
coupling agent (i.e., vinyl amine-based polymer) was combined with
MAPP [116]. The cationic polymer–bearing amino groups can react with
MAPP, forming hydrogen bonds with cellulose. When a combination of
MAPP and a cationic polymer was added, the PP composite with 30 wt %
Kraft pulp had a 27% higher tensile strength and an 18% higher modulus
than the composite with MAPP only.
4.5. Emergence of additive manufacturing of NFRCs
Additive manufacturing, or 3D printing, has recently been notably
expanded to revolutionize the conventional manufacturing process
across many industries. Compared with the traditional composite mak­
ing processes mentioned previously, 3D printing has several advantages,
including quick and easy manufacturing, reduced limitation on com­
posites geometry, increased controllability of fiber volume and direc­
tion, reduced thermal degradation or deconstruction of natural fiber,
and saving of expensive molds and tools. Considerable research has been
conducted using forestry and agricultural fibers as 3D printing feed­
stock, such as microfibrillated cellulose and nanocellulose [117,118].
Fused deposition modeling (FDM) is one of the simple and widely used
3D printing techniques because of the wide range of available polymers,
such as PLA, polycaprolactone, and acrylonitrile butadiene styrene. In
FDM, material filament consisting of fiber and matrix is guided through
a heated nozzle with a feeding roller, and the melt paste is deposited
layer by layer on a printing platform according to a computer-designed
architecture and process (Fig. 8a). The partially liquefied layer is then
fused with the previous layer when the material solidifies during
cooling.
Micro- and nanocellulose have been incorporated into PLA for
fabricating 3D printing filament and composites. Microcellulose/PLA 3D
printing filament has been produced using solvent casting followed by
twin-screw extrusion of PLA with the addition of a small amount of
microcellulose (<5 wt %) [121]. However, this process results in higher
moisture uptake of the microcellulose/PLA filament. Additionally, it has
a potential risk of forming bubbles in the filament as a result of the
addition of microcellulose, although this risk can be reduced by opti­
mizing the extrusion parameters. Recently, Tekinalp et al. used a similar
process to make CNF/PLA filament for 3D printing [122]. The me­
chanical properties of the 3D printed composites were compared with
those made from the traditional compression molding process. At 30 wt
% CNF content, the 3D printed sample showed a significantly higher
elastic modulus of 7.12 GPa and storage modulus of 1.72 GPa than the
compression-molded sample of 6.57 and 0.9 GPa, respectively. The
authors proposed a “microsponges” reinforcing mechanism in which the
polymer penetrating the freeze-dried CNF porous network during
melt-processing creates mechanical interlocking between the CNF and
matrix. The higher modulus of 3D printed samples was explained by the
higher crystallinity due to an extended temperature being maintained
during the printing process, and the possible orientation of CNF bundles
along with the printing direction. Although the tensile strength of the
printed sample had a remarkable increase up to 80% compared with
neat PLA, the mechanical performance of printed composites was infe­
rior to the composites made from compression. This was attributed to
the presence of porosity/defects in the printed sample, which can be
improved by optimizing the printing conditions (e.g., increased bed
temperature for good fusion and lower extrusion temperature for pore
reduction).
A commercially available FDM 3D printer was modified with two
separate filament supplying paths for polymer matrix and reinforcing
fiber, respectively (Fig. 8b), allowing the production of continuous
NFRCs by in-nozzle impregnation [119]. Composites with ~6 vol % jute
yarn or carbon fiber were successfully fabricated. The printed jute/PLA
had a 134% higher tensile strength and 157% higher modulus than the
neat PLA, while the carbon/PLA composite showed much more
improvement, 435% and 599%, respectively. Comparable and even
superior tensile properties of 3D printed composites can be achieved in
comparison with the values of most non-fabric fiber–reinforced PLA (as
shown in Fig. 4). With only 6.1 vol % of natural fiber, the tensile
properties of this printed jute/PLA composite were close to the 20 wt %
glass fiber–reinforced PLA [44], even though the performance of the
printed jute/PLA composite was thought to be not maximized because
the jute yarn was fed into the nozzle with no tension. The fibers without
tension could lead to a nonuniform configuration of the twisted jute yarn
fiber, resulting in weak points in the printed specimen. Overall, this
technique enables direct 3D printing of continuous fiber composites that
will substantially expand the methodology of 3D printing for NFRCs
with high mechanical performance.

10
M. Li et al.
Fig. 8. Schematic of FDM process (a) [119] and the FDM-based 3D printer head used to produce continuous fiber–reinforced composite using in-nozzle impregnation
(b) [120].
Hinchcliffe et al. demonstrated a technique combining 3D printing
and fiber prestressing for high-performance NFRCs [123], which can
partially address the lack-of-tension disadvantage observed in the above
continuous-fiber composite fabrication. The 3D printed PLA specimen
was first prepared with and without post-tensioning ducts. Then, flax
and jute fiber strands were threaded through the ducts, stressed to
prescribed levels of pretension, and affixed into place using anchors. The
measured tensile and flexural properties were transformed into specific
mechanical values (e.g., tensile or flexural properties to weight ratio).
The results indicated that the reduction in material quantities from ducts
showed superior specific mechanical properties. Prestressing of flax fi­
bers threaded in the duct further increased the specific tensile strength
and modulus compared with the no-duct PLA specimen. However, this
technique showed several shortcomings, including that it (1) is only
suitable for high-density matrices (e.g., PLA and HDPE), (2) requires
consistent fiber mechanical properties (e.g., fiber strands rather than
single fiber), (3) needs complicated designing of duct, and (4) has fiber
prestressing loss from loosening anchorage.
Manipulation of the hygroscopic and anisotropic feature of natural
fiber leads creatively to a concept of 4D printing of NFRCs, which refers
to the responsive capability of 3D printed materials to actuate under an
external stimulus. The moisture adsorption of natural fiber has histori­
cally been thought to be one of the limitations of the applications of
NFRCs. However, this inherent hygroscopic fiber transformation and
anisotropic properties have been recently combined with 3D printing
technologies for the development of programmable material and
responsive architectures [124]. The hygroscopic property of wood fiber
enables the composite’s structural transformation in response to envi­
ronmental changes (e.g., temperature, humidity, light radiation), and
the integrated anisotropic cell wall structure and 3D printing patterns
allow precise control over the directions and degrees of deformation (i.
e., curling). Correa et al. demonstrated that self-transformable com­
posites can be fabricated using wood fiber and acrylonitrile butadiene
styrene or nylon fiber [124]. After exposure to moisture by water sub­
mersion or water vapor, the 3D printed wood composites started curling
in a programmed way based on the designed architecture of the com­
posites and the controlled climatic conditions. This curling actuation
behavior was found to be fully reversible for more than 30 cycles
without any visible defects or changes in curling range. Another study of
wood fiber biocomposites found that the printing directions (i.e., 0◦ and
90◦ ) and printing width significantly influenced the hygromorphic
11
Composites Part B 200 (2020) 108254
dynamic of the biocomposite because of their differential micro-porous
structure [125]. Manipulation of the differential composite micro­
structure and the anisotropic hygro-elastic and swelling properties
enabled a controlled self-actuating functionality of the printed bilayer
wood fiber biocomposites (Fig. 9). The printed bilayer structure was
obtained by tailoring the printing directions consisting of an active layer
with high radial swelling printed at 0◦ and a passive layer with low axial
swelling at 90◦ (Fig. 9a). The printed biocomposites actuated in response
to the external stimulus: hygromorphic bending after immersion in
water (Fig. 9b and c). Because the microstructure associated with
varying porosity determines the water update and swelling behavior, it
therefore alters the actuation response. However, the transformation
process of the biocomposites in this study was not fully reversible.
Together, taking advantage of the inherently hygroscopic and aniso­
tropic properties of natural fiber and the multi-material and tunable
microstructure with 3D printing technologies, high-performance NFRCs
with programmable moisture-actuated functionality can be generated.
4.6. Exploration of new natural fiber sources
A great variety of new plant-based natural fibers and their rein­
forcing performance for polymer composites have been explored
(Table 4). Comprehensive characterization of these newly emerged fi­
bers has shown feasible physical, mechanical, thermal, and morpho­
logical features as alternative reinforcing natural fibers. A common
theme involved in the performance of NFRCs is the chemical, structural,
and morphological characteristics of natural fiber. In general, crystalline
cellulose content and its microfibril alignment with the fiber axis are
positively correlated with the tensile properties of the fiber, whereas the
hemicellulose and lignin content correspond to low-stress values and
increased moisture absorption and failure strain [126–128]. However, a
few other studies have observed positive effects for lignin-containing
fibers on the photochemical aging and weathering withstanding of
certain NFRCs testing [129–131].
5. Life cycle assessment
Natural fiber composites may have lower environmental impacts
than glass- or carbon-fiber composites if their production impacts are
sufficiently low or if they improve the environmental performance of the
product.
M. Li et al. Composites Part B 200 (2020) 108254

Fig. 9. 3D printed hygromorph bilayer wood fiber/PLA/PHA composites. (a) Principle of hygromorph biocomposite design based on the bioinspiration paradigm.
Example of hygromorph biocomposite made by FDM (b) before and (c) after immersion. Reproduced from Ref. [125] with permission from Elsevier.

Table 4
Properties of recently emerged natural fibers and their reinforced composites.
Fiber source (or type) Status of fiber (d)/composite (conc., matrix) Density (g/cm3) σ (MPa) E (GPa) Elong. (%) Ref.

Agave tequilana Cooked (329–426 μm) 0.88 42–58 2.6–2.9 11–15 [132]
Injection-molded random fiber (30%, PP) — 29 → 32 1.53 → 2.48 —→4.8 [27]
Althaea officinalis Solvent and water retted (156–194 μm) 1.2 415 65.4 3.9 [133]
Areca fruit fiber Water retted (400–500 μm) 0.7–0.8 147–322 1.1–3.2 10–13 [134]
Random fiber sheet (40%, polyester) — 37 → 68 1.5 → 1.3 —→5.2 [134]
Arundo donax Stripped (500 μm) 1.2 222 8.6 2.6 [135]
Hand layup chopped (5%, epoxy) — 53 → 74# 1.7 → 3.1# 7→— [136]
Cissus quadrangularis Water retted (198 μm) 1.2–1.5 207–322 5.6–6.3 5.2 [137]
Random fiber sheet (40%, polyester) — 19 → 36 0.9 → 2.2 —→4.9 [138]
Conium maculatum Water retted (200 μm) — 328 15.8 2.7 [139]
Cortaderia selloana Random fiber (15%, bio-PE) — —→20 —→0.5 —→1.5 [140]
Cynara cardunculus Water retted (300 μm) 1.6 201 11.6 3 [141]
Unidirectional (10%, PLA) 1.6 47 → 50 3.2 → 4.5 2.5 → 1.4 [142]
Dichrostachys Cinerea Water retted 1.2 873 — — [143]
Dracaena reflexa Water retted (176 μm) 0.79 830 46.4 2.9 [144]
Fimbristylis globulosa Water retted (34 μm) 0.9 452 17.4 — [145]
Furcraea foetida Water retted (13 μm) 0.8 ~600 6.0–6.5 10.5 [146]
Heteropogon Contortus Manually plucked 0.6 476 48 1.6 [147]
Ishinosiphon koern Retted (280 μm) 0.57 614 21 — [148]
Juncus effusus Retted (280 μm) 1.1 113 4.4 2.8 [149]
Lygeum spartum Retted (180–433 μm) 1.5 65–280 4.5–13.3 1.5–3.7 [150]
Manicaria saccifera Bracts (100 μm) 0.8–1.1 255–391& 1.8–2.4 5.0–5.4 [151]
Natural fabric (40%, PLA) 0.8–1.1 54 → 68 3.2 → 4.9 4.9 → 3.5 [37]
Okra Random fiber (15%, cornstarch, 90 μm) — 11 → 18 0.5 → 1.6 5.1 → 2.6 [152]
Pennisetum purpureum Water retted (150–250 μm) 0.4 73 5.7 1.4 [153]
Random fiber (25%, polyester) — —→16 —→3.0 — [154]
Ricinus communis Alkaline retted (20–80 μm) — 493 20.9 3.0 [155]
Carded fiber mat, PP (50 wt %) — 24.1 0.92 — [155]

d: diameter; σ: tensile strength; E: elastic modulus; elong.: elongation at break; —: data not reported; & denotes cN/m; # denotes flexural strength; → shows the strength
changes from neat polymer to reinforced composite.

An LCA concluded that NFRCs can provide significant energy savings
and greenhouse gas reduction when used to reduce the weight of
aircraft, trucks, automobiles, and other vehicles. These energy savings
from light-weighting are larger than the impacts of fiber production.
Even so, the impact of natural fiber production is an area that would
benefit from further research because agricultural processes used to
produce fibers can have significant impacts [156]. Another LCA study of
comparing a 3 kg 30% glass-fiber composite component with a 30%
cellulose-fiber component and a 40% kenaf-fiber component in auto­
motive applications found that the environmental benefits of NFRCs are
primarily because NFRCs are lighter than glass-fiber composites and
therefore increase the energy efficiency of automobiles [157]. Across the
fibers, the 3-kg part had a life-cycle energy consumption of
approximately 20 MJ for fiber production, 150 MJ for resin production,
80 MJ for part manufacturing, 20 MJ for sourcing, 1200 MJ for use, and
1 MJ for end of life, and 1450 MJ for total life-cycle energy consumption.
Life-cycle energy consumption is largest for the use-phase because in
this application, the composite is part of an automobile, so the use-phase
energy consumption is proportional to the weight of the component. The
cellulose- and kenaf-fiber components weigh less than the glass-fiber
component, so the use-phase energy is lower. All the options had
approximately the same life-cycle energy for the sum of the fiber pro­
duction, resin production, part manufacturing, sourcing, and end of life,
with the result that the life-cycle energy differences came down to the
use-phase and the lightest composite had the lowest impact. The kenaf
composite and the cellulose composite provided about 7% reduction in

12
M. Li et al. Composites Part B 200 (2020) 108254

Table 5
Automobile companies using natural fiber–reinforced composites [6,166,168,169,177,178].
Automobile Natural fibers Applications

Audi Flax, sisal Seat back, side and back door panel, boot liners, hat rack, spare tire liners
BMW Flax, sisal, wood, cotton, bast Door panels, headliner panels, boot liners, seat backs, noise insulation panels, molded foot well liners, bumpers, fender liners,
shields
Brazilian Jute coir Trim parts, seat cushions
trucks
Chevrolet Flax Trim panels
Impala
Citroen Vegetable, wood Interior door paneling, parcel shelves, boot liners, mudguards
Daimler-Benz — Door panels, windshields, dashboards, business tables, pillar cover panels, glove boxes, instrumental panel support,
insulation, molding rods/apertures, seat backrest panels, trunk panels, seat surface/backrests, internal engine covers, engine
insulation, sun visors, bumpers, wheel boxes, roof covers
Daimler Coir, cotton, flax, hemp, sisal, Door panels, engine and transmission covers, pillar cover panels, windshields, dashboards, business tables
Chrysler abaca
Fiat Bamboo Door panels
Ford Kenaf, hemp, rice hulls, tomato, Floor trays, door panels, B-pillars, boot liners, wiring brackets, storage, front grills
wheat straw
General Motors Flax, hemp, kenaf Seat backs, inner door panels, cargo area floors
Honda — Cargo area
Lotus Hemp, sisal, kenaf Body panels, spoilers, seats, interior carpets
Mercedes-Benz Hemp, sisal, flax, cotton, banana Inner door panels, door panels, rear panel shelves, engine encapsulation, trunk covers
Abaca, flax, sisal, wood Door panels, engine encapsulation, spare wheel pan covers, door liners, seat backrests, parcel shelves, trunk covers
Mitsubishi Bamboo, flax, hemp, cotton Cargo area floors, door panels, instrumental panels, floor mats
Opel — Instrumental panels, headliner panels, door panels, pillar cover panels
Peugeot — Front and rear door panels, seat backs, parcel shelves
Renault — Rear parcel shelves
Rover — Insulation, rear storage shelves/panels
Saturn — Package trays and door panels
Toyota Kenaf, sugar cane, sweet potato Door panels, seat backs, floor mats, spare tire covers, package shelves
Kenaf Spare tire covers
Vauxhall — Headliner panels, interior door panels, pillar cover panels, and instrument panels
Volkswagen Flax, sisal Door panels, seat backs, boot-lid finish panels, boot liners
Volvo Hemp, jute, rapeseed, wood Seat padding, natural foams, cargo floor trays, dashboards, ceilings

—: not reported.

Fig. 10. Mercedes-Benz components containing natural fibers (flax, hemp, sisal, wool, and others) of model (a) A-class, (b) C-class, (c) E-class, and (d) S-class.
Reproduced from Ref. [17,166,169], with permission from John Wiley for (a), (b), and (d), and Springer for (c).

13
M. Li et al. Composites Part B 200 (2020) 108254

Table 6
Applications of natural fibers composites in several fields.
Fibers Other major compositions Potential applications Ref.

Civil Construction
Banana Soil, cement Compressed earth block [180]
Curaua, jute, sisal, ramie, pineapple Cement, metakaolin, fly ash Cementitious materials [181,182]
Flax, jute, sisal, hemp, coir, oil palm Polyester, epoxy, mortar Masonry [183–189]
Jute Glass fiber, vinyl ester Deck panel [190]
Kenaf Plaster of Paris Ceiling [191]
Wheat straw, corn husk, — Thermal insulation materials [192]
Wood, cellulose, cork — Thermal insulation materials [193]
Furniture and Architecture
Lignocellulose, straw HDPE Plus lounge furniture [194]
Hemp Epoxy Hemp chair furniture [194]
Hemp, flax Polyethersulfone Ignot bio- and Polycal acoustic [194]
panel
Lignocellulose Thermoplastic, thermoset resin BioMat research pavilion [194]
Sports and Clothes
Cotton, hemp, jute, bamboo, sugarcane bagasse, coconut, Polyester Footwear [195]
banana, raffia
Curaua Aluminum/graphene oxide, epoxy Ballistic armor materials [196,197]
Flax, hemp Epoxy Racing bicycle [198]
Flax Carbon fiber, epoxy Bicycle frame [199]
Jute Polyester Winter over coat [200]
Jute, sisal, coconut, areca, banana Epoxy Helmet shell [201]
Kenaf Kevlar, epoxy Ballistic armor materials [202,203]
Kenaf PLA Mobile phone casing [198]
Kenaf, pineapple, mengkuang Epoxy Recurve bow [204]
Oil palm empty fruit bunch Epoxy Sports utility [205]
Aerospace
Hemp Epoxy Electronic racks for helicopter [206]
Ramie Matrix Aircraft wing boxes [207]
Kenaf Glass fiber, matrix Aircraft materials [207]
Biomedical and Pharmaceutical
Cotton Epoxy Medical imaging [208]
Cotton, sugarcane PLA, starch Drugs, antibiotics [209]
Coconut, sugarcane Oregano oil, poly(3-hydroxybutyrate-co-3- Antimicrobial, antibiotics [209]
hydroxyvalerate), starch
Flax, ramie Epoxy Bone grafting, orthopedic [210]
implants
Hemp, sisal, coir Polycaprolactone Orthoses materials [211]
Jute PP Enzyme [209]
Jute, sugarcane, flax, cotton, kenaf, bamboo Plant extracts, polyester, PP, chitosan Biomedical nanoparticles, [209]
antibiotics
Sisal Poly(methyl methacrylate) Drug delivery [209]
Others
Bamboo PLA Packaging [212]
Alpha, banana, bamboo, cotton, flax, jute, kenaf, oil palm, Polyester, PP, PE, PLA, epoxy, rubber, polyurethane, wheat Dielectric materials [213,214]
sisal gluten
Flax Carbon nanotube Electrodes [215]
Flax, jute, coir, sisal Glass fiber, epoxy Wind turbine blades [216]
Flax, seagrass Glass fiber, polyhydroxyalkanoates, epoxy Marine materials [217,218]
Jute Glass fiber, polyester Solar parabolic trough collector [219]
Jute, flax, kenaf, hemp Aluminum, epoxy, polyester Electromagnetic interference [220,221]
shields
Wood cellulose Cobalt sulfide, carbon fibers Battery [222]

—: not reported.

life-cycle energy use of the component, compared with the glass-fiber
composites, with potential as high as 19% with resizing of the power
train.
Landfilling, incineration with energy recovery, and recycling are
three end-of-life options that have been considered [158]. Most fiber­
–reinforced polymers, including both carbon and glass fibers as well as
natural fibers, are landfilled. Landfilling of biomass sequesters carbon,
providing a greenhouse gas reduction; incineration with energy recov­
ery releases the carbon in the biomass but can partially displace the use
of fossil fuels, providing an alternative route to greenhouse gas reduc­
tion. The amount of energy recovered from the incineration of NFRCs
ranged from 12 to 34 MJ/kg of the composite, which is more than for
glass fiber composites, which are around 7.5 MJ/kg [156].
Hedlund-Åström studied the end of life of polymer composites and found
environmental benefits both for recycling of the flax/PP composite and
for incineration for energy content if the process would replace coal
combustion [159]. The option of making pellets from the waste NFRCs
and combusting them for energy recovery was also considered but was
more expensive than the direct waste incineration option. The overall
implication of LCA of NFRCs, which have been mostly focused on
automotive applications, is that the benefits are mainly due to their light
weight rather than their natural origin.
Several studies, however, have pointed out that NFRCs can have
inferior environmental impacts than alternatives when certain factors

14
M. Li et al.
are considered. For example, flax is superior in most environmental
impact categories compared with glass fiber, except for eutrophication,
because of the use of fertilizers for flax production [160]. This is one of
the few studies to examine the potential for eutrophication, and it sug­
gests that other fibers produced with fertilizers may have similar im­
pacts. In a cradle-to-manufacturing LCA, Rodriguez et al. suggested that
the use of the banana fiber required changes in the composite to achieve
the same functional characteristics, in some cases eliminating the pro­
duction advantage of natural fiber [161]. Additionally, the fiber treat­
ment method played a vital role in the analysis of the environmental
impact of NFRCs [162]. The analysis showed that human health,
ecosystem, and resource impacts are mostly independent of whether
glass or hemp is used as the reinforcing material in both the reinforced
PP or PLA composites [163].
Building on the understanding of the design and production of
NFRCs, the lifecycle environmental effects of design requirements have
been evaluated. A flax-fiber mat with design optimization for stiffness
equal to a glass-fiber mat provides energy savings in automotive uses
because the flax fiber mat is lighter. In contrast, in an injection-molded
application requiring equal stiffness, even an optimized design for the
flax-fiber composite has approximately the same mass and very similar
impact as the glass fiber counterpart [164]. Further studies that incor­
porate the advancing knowledge of natural fiber composite
manufacturing and design hold promise for illuminating the interplay
between improved physical and environmental performance. Life-cycle
costing and social impact measures are emerging that have the potential
to provide a more holistic sustainability assessment for natural fiber
composites [165].
6. NFRC applications
NFRCs has been widely applied in the automotive sector. It has been
estimated that 75% of fuel consumption directly relates to vehicle
weight, with every 10% reduction in vehicle weight resulting in 6–8%
increment in fuel economy and every 100 kg in weight saving in auto­
motive, leading to approximately 20 g/km reduction in CO2 emission of
commonly used powertrains [2]. Weight reduction directly supports the
European Commission’s and the European Automobiles Manufacturers
Association’s goal of reducing CO2 emission [166,167]. The European
Union End-of-Life Vehicle Directive (European Directive 2000/53/EC)
has targeted reuse or recycling 95 wt % of vehicles starting in 2015. In
the United States, the Corporate Average Fuel Economy standards
require that automakers increase the fuel economy of cars and light-duty
trucks to 54.5 mpg by 2025 [27]. Similar regulations have been adopted
in many other countries to increase the fuel economy and CO2 reduction
[167].
Early efforts directed at using bio-based materials in vehicle parts
were contemplated by Ford Motor Company dating back to the 1930s,
and there are several highlighted applications of NFRCs in the auto­
motive industry to date [166,168]. For example, in 2000, Audi launched
the A2 midrange car in which the door trim panels were made of
flax/sisal–reinforced PU and Mercedes-Benz disclosed a flax/polyester
engine and transmission enclosures for the first time for standard exte­
rior components. By 2019, Porsche announced that the 718 Cayman GT4
Clubsport racecar was the world’s first vehicle with bodywork built from
hemp/flax–reinforced composites. In the past decades, European and
North American governmental legislations have encouraged the appli­
cations of NFRCs in the automotive sector. These “green” composites
derived from natural fibers are increasingly and extensively applied in
automotive parts by manufacturers and suppliers, such as door panels,
seat backs, headliners, trays, dashboards, and interior parts (Table 5).
Among these abundant NFRCs, flax–-, hemp–, kenaf–, and
sisal–reinforced thermoplastics have dominated for automotive
15
Composites Part B 200 (2020) 108254
component applications. All the major car manufacturers such as Audi,
BMW, Daimler Chrysler, Ford Motor Company, General Motors,
Mercedes-Benz, and Toyota have used bio-based composites in various
applications. For Mercedes-Benz, natural fibers have been extensively
applied in components of various models (Fig. 10) [169]. For example,
~20.8 kg of natural fibers (wood, banana, and flax) in more than 20
components are used for the A-class; ~19.8 kg of natural fibers (wood,
coconut, and honeycomb cardboard) in more than 21 components for
the B-class; ~17 kg of natural fibers (honeycomb cardboard, charcoal
coke, sisal, wood, cotton) in more than 27 components for the C-class;
~21 kg of natural fibers (jute, flax, hemp, sisal, and olive coke) in more
than 44 components for the E-class; and ~43 kg of natural fibers in more
than 27 components for the S-class. BMW has been using NFRCs since
the early 1990s in M3, M5, and M7 series models with up to 24 kg of
renewable materials being used.
Generally, NFRCs are primarily used in interior automotive parts
because of their intrinsic moisture sensitivity and relatively low me­
chanical properties. Many nonstructural interior parts, such as indoor
panels, dashboard, seat backs/fillers/liners, floor mats, package shelves,
and storage bins, can include NFRCs. Examples of NFRCs used for
exterior components in a production vehicle include flax/polyester
composites in the engine and transmission enclosures for sound insu­
lation, abaca–reinforced composites for the spare tire well covers, fender
components, spoilers, bumpers, seat frame, and load floors. Recently,
new studies on NFRCs, such as flax/Acrodur with impregnated flax tape
at short crosslinking times for fast molding parts in vehicles [170],
flax/vinyl ester composites for automobile hoods [171], hemp/PP
composites resisting weathering for interior and decking components
and small auto parts [172,173], kenaf/epoxy composites for spall liners
[81,82], maple and pine flour–reinforced Nylon 6 with enhanced ther­
mal stability for under hood parts [174], palm kernel shell fiber/­
phenolic resin for brake pads [175], and bamboo/polyurethane
composites for sound absorption materials for door panels [176] have
expanded the potential automotive applications of NFRCs. Research and
development to advance the applications of NFRCs to more structural
components are desirable.
Due to the light weight, low thermal conductivity, and low envi­
ronmental impacts of renewable materials, NFRCs have also been
advanced recently for their applications in masonry, soil blending,
cementitious materials, thermal insulating materials, furniture, and
decks applied in the civil construction, furniture, and architecture
(Table 6) [179]. However, such composites are generally limited to thin
sheet applications with high fiber volume fraction, making them not
particularly useful for general construction purposes. Recently, natural
fiber composites have been investigated with potentially extensive ap­
plications in several other areas, such as sports, clothes, recreation
equipment, aerospace, biomedical and pharmaceutical, electrical,
packaging, and electromagnetic applications (Table 6).
7. Summary and outlook
NFRCs have well-known appealing characteristics, such as light
weight, environmental friendliness, recyclability, and achievable me­
chanical performance derived from natural fibers. Applying NFRCs,
primarily in the automotive sector, can provide weight reduction, en­
ergy efficiency, environmental safety, and health benefits. However, the
innate heterogeneous characteristics and hydrophilicity of natural fibers
raise challenges to the manufacturing and application of NFRCs. The
critical issues are fiber quality inconsistency, poor fiber/matrix adhe­
sion, hard fiber dispersion, limited composite manufacturing conditions,
and moisture absorption. Exploration of new natural fiber with abun­
dance can diversify fiber sources and reduce material cost. However,
consistent quality of natural fibers is always an important feature for a
M. Li et al.
steady performance of NFRCs. Research on the fundamental under­
standing of the microstructure of the interphase is critical to further
improve natural fibers’ dispersion and interfacial bonding with polymer
matrices and the mechanical properties of NFRCs. Coupling agents and
chemical modification can significantly improve the compatibility of
natural fiber and polymer matrix, but the interfacial bonding strength
seems to play a larger role given the thermo-mechanical orthotropicity
of the fiber. In turn, unidirectional fiber, mat fabric stacking, hybridi­
zation, and processing revolution strategies can substantially impart the
longitudinal performance of fiber into NFRCs. Particularly, natural fi­
bers with superior strength and modulus, such as nano-scaled cellulosic
fibers, have emerged and could play a pivotal role as new reinforcing
components for polymers. Additionally, the 3D printing of NFRCs with
the capability of complex structural design and advanced actuation
performance can potentially transform and expand the application of
NFRCs significantly in the future. The future market of NFRCs is
increasing, and their application, particularly in automotive, civil en­
gineering, sports, and biomedical sectors, is quite promising.
Declaration of competing interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
Acknowledgments
This research was funded by the US Department of Energy under
contract DE-FOA-0001232. Oak Ridge National Laboratory is managed
by UT-Battelle, LLC under Contract DE-AC05-00OR22725 with the US
Department of Energy (DOE). The views and opinions of the authors
expressed herein do not necessarily state or reflect those of the United
States Government or any agency thereof. Neither the United States
Government nor any agency thereof, nor any of their employees, makes
any warranty, expressed or implied, or assumes any legal liability or
responsibility for the accuracy, completeness, or usefulness of any in­
formation, apparatus, product, or process disclosed, or represents that
its use would not infringe privately owned rights. ML also acknowledges
the support from the University of Tennessee Institute of Agriculture and
the University of Tennessee Agricultural Experiment Station and
AgResearch.
Appendix A. Supplementary data
Supplementary data to this article can be found online at https://doi.
org/10.1016/j.compositesb.2020.108254.
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