REVIEW

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Varied Alignment Methods and Versatile Actuations for

Liquid Crystal Elastomers: A Review
Jiayou Zhao, Limei Zhang, and Jian Hu*

biomedicine,[30,31] flexible electronics,[32,33]

Liquid crystal elastomers (LCEs) are a class of programmable polymer materials light energy collection,[34] etc.
that can deform reversibly under diverse stimuli such as light, heat, electric field, LCEs are composed of rigid mesogens
and magnetic field. LCEs have demonstrated their potential applications in and flexible polymer networks, with the
result that the anisotropy of liquid crystal
soft robots, soft actuators, artificial muscles, etc. How to align the mesogen
and the rubber elasticity of polymer net-
orientation and achieve actuations of LCEs are the two most important issues for work can be both shown in LCEs.[35–37]
the studies on LCEs. At present, varied alignment methods and versatile Induced by mechanical stress, external
actuations for LCEs have developed rapidly. However, few reviews are addressing field, or surface effect, the long axes of
these two important issues simultaneously. In this review, three types of the mesogens can be aligned into specific
directions (expressed by the director n),
alignment methods for LCEs as mechanical stress-induced alignment, external
and this process is called alignment.
field-induced alignment, and surface effect-induced alignment are summarized, Liquid crystal polymers after alignment
and comparing their programmability toward the mesogen orientation is focused are chemically[38] or physically[39] cross-
on. The key factors influencing the versatile actuations of LCEs are their linked to form anisotropic monodomain
orientation structure (intrinsic factor) and the applied external stimuli (extrinsic (including nematic, smectic, or cholesteric)
factor). Thus, actuations are classified into two types on the basis of pro- LCEs. On the contrary, LCEs are in a poly-
domain state with isotropy when the direc-
grammable orientation structure and selective external stimuli, respectively,
tors of liquid crystal domains are arranged
and focus on comparing their deformation controllability. Finally, an outlook for disorderly. Triggered by the external physi-
the future key technologies to develop versatile, precise, and fast-responsive cal or chemical stimuli, the response and
deformation actuations for LCEs is proposed. deformation originated from the phase
transition from a liquid crystalline phase
to an isotropic phase is significantly
enhanced in the monodomain LCEs. This
process is macroscopically manifested as the size shrinkage of
1. Introduction LCEs in the orientation direction.[40,41] Therefore, the orientation
degree of LCEs affects the maximum deformation actuated by
Liquid crystal elastomers (LCEs) are a class of polymer materials
[1,2] the external stimuli to a large extent, whereas the orientation direc-
that can produce reversible strain responses under heat,
tion of LCEs determines their macroscopic deformation direction.
light,[3–6] electric field[7] (or electric induction heat),[8,9] magnetic
The programmability of the mesogen orientation lays a foundation
field (or magnetic induction heat), [10,11]
moisture,[12]
or sol-
[13] for achieving versatile deformation actuations of LCEs.[42] Aligning
vent, etc. They have attracted intense attention due to their
the mesogen orientation and achieving versatile actuations of LCEs
enormous potential applications in soft robots,[1,9,14–18] soft
are always the central research objects in the field of LCEs, and
actuators,[4,8,14,19–23] sensors,[22,24–26] artificial muscles,[27–29] have developed rapidly in recent years. However, few reviews
are addressing these two important issues simultaneously.
Herein, in Section 1, we briefly elucidate the relationships
J. Zhao, L. Zhang, J. Hu between the microscopic orientation structure of LCEs, external
State Key Laboratory for Strength and Vibration of Mechanical Structures,
stimuli, and macroscopic deformation characteristics of LCEs.
School of Aerospace Engineering
Xi’an Jiaotong University In Section 2, we introduce three types of LCE alignment
Xi’an 710049, China methods and their basic principles, and focus on comparing their
E-mail: hujian@mail.xjtu.edu.cn programmability toward the mesogen orientation. In Section 3,
The ORCID identification number(s) for the author(s) of this article we summarize two types of actuations for LCEs on the basis of
can be found under https://doi.org/10.1002/aisy.202100065. the latest development, and focus on comparing their deforma-
© 2021 The Authors. Advanced Intelligent Systems published by Wiley-
tion controllability. In Section 4, we propose an outlook for the
VCH GmbH. This is an open access article under the terms of the future key technologies to develop versatile, precise, and fast-
Creative Commons Attribution License, which permits use, distribution responsive deformation actuations for LCEs. This review aims
and reproduction in any medium, provided the original work is to help people to design and prepare LCEs with programmable
properly cited. orientation structure and excellent actuation characteristics, and
DOI: 10.1002/aisy.202100065 promote their practical development.

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2. Alignment Methods for LCEs
The mesogen orientation is the basis for the macroscopic defor-
mation of LCEs. Varied alignment methods have been developed
to align the mesogen orientation. In this review, the alignment
methods for LCEs are divided into three categories according to
alignment inducement, including mechanical stress-induced
alignment, external field-induced alignment, and surface
effect-induced alignment. Different alignment technologies are
shown in Table 1 and compared in terms of alignment direction,
programmability, and limiting factor.
2.1. Mechanical Stress-Induced Alignment
The long axes of mesogens can be aligned parallel or perpendic-
ular to mechanical stress, which is the basic feature of mechani-
cal stress-induced alignment. The main stress types to induce
alignment are tensile stress, compressive stress, and shear stress.
In some cases, multiple stresses are coupled together. According
to the stress types, we introduce the mechanical stress-induced
alignment technologies separately in the following paragraphs.
Tensile stress induced-alignment has been widely used for
LCEs because of its simple operation and excellent alignment
effect. The most common technology is the uniaxial stretching
in the procedure of a two-step crosslinking reaction (Figure 1A),
which was first proposed by Finkelmann and co-workers[38] and
further developed by Bowman and co-workers.[43] Generally,
a weakly crosslinked LCE is prepared in the first-stage
reaction,[38,43–46] followed by a mechanical stretching operation
immediately. Subsequently, the second-stage reaction is carried
out to fix the alignment of LCEs. In recent years, Ji and co-work-
ers fabricated novel LCEs with exchangeable dynamic covalent
bonds.[47] In these material systems, the alignment of LCEs
can be achieved after fully curing,[2,48] different from that in
the two-step reactions. When uniaxial tensile stress reaches a
threshold value, the deviation angle between the long axes of
the mesogens and the direction of stress rapidly reduces,
enabling the orientation degree of LCEs to raise sharply.[37,49]
The uniaxially aligned LCEs show the unidirectional orientation

Table 1. Alignment methods for LCEs.

Alignment Alignment Alignment technology Alignment direction Programmability Limiting factor Illustration
method inducement
Mechanical Tensile stress Uniaxial stretching The stretching direction
Fracture strength[128] Figure 1A
stress-induced Multiaxial stretching The stretching directions
Fracture strength[128] Figure 1B
alignment
Uneven alignment[50]
Compressive stress Anisotropic deswelling Perpendicular to the
Deswelling ratio Figure 1C
compression axis[51]
p [55,59]
Shear stress 4D printing The direction along the Printing precision[59,100] Figure 1D
printing path[59]
Microfluidic alignment Parallel to the direction of
Capillary channel size[62,126] Figure 1 E
flow[126]
Fiber electrospinning or The direction along the
The final diameter of Figure 1 F
drawing fiber[64] fibersa)[64]
p[67,68,94]
Multiple stresses Stamping, crimping, and The direction of stress Fracture strength[128] Figure 1G,H
embossing
p [130]
External field- Magnetic field Magnetic field-induced The direction of magnetic Magnetic induction Figure 2A
induced alignment induction intensity[70,129] intensity[79]
alignment p[131]
Electric field Electric field-induced The direction of the electric Electric field intensity[69] Figure 2B
alignment field b)[71–73]
p [132,133]
Light Photoalignment Perpendicular or parallel to Wavelength of light,[105] laser Figure 2C
the direction of the light beam power density[34]
vector[77]
Surface Intermolecular force Alignment template The direction of friction[22]
Static charge and scratches Figure 3B
effect-induced and microchannel prepared by rubbing that are not parallel to the
alignment alignment direction[134]
p[83]
Alignment template prepared The direction of The size of microchannels[83] Figure 3C
by photolithography microchannels[83]
Alignment template from The stretching direction of
The porous density of Figure 3D
anisotropic porous materials anisotropic pores[86] alignment templates
Alignment template from Parallel to the CNT-aligned
Orientation degree of CNT Figure 3E
oriented CNTs direction[87] arrays

a)
The final diameter of fibers is affected by the intrinsic properties of the polymer solution and operating conditions; b)For smectic liquid crystals, a tilt angle can be induced by
an electric field, which is known as the electroclinic effect.

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Figure 1. Schematic diagrams of various mechanical stress-induced alignment methods. A) Aligning LCEs by uniaxial stretching. Reproduced with per-
mission.[43] Copyright 2015, RSC Publishing. B) Aligning LCEs by multiaxial stretching. Reproduced with permission.[50] Copyright 2015, Elsevier.
C) Aligning LCEs by anisotropic deswelling. D) Aligning LCEs by 4D printing. Reproduced with permission.[55] Copyright 2017, American Chemical
Society. E) Aligning LCEs by microfluidic technology. (i) Schematic diagram; (ii) flow profile; (iii) director configuration in the core–shell particles.
Reproduced with permission.[126] Copyright 2012, Springer Nature. F) Aligning LCE fibers by drawing. Reproduced with permission.[27] Copyright
2019, American Chemical Society. G) Aligning LCEs by stamping, crimping, and embossing. Reproduced with permission.[68] Copyright 2019, Royal
Society of Chemistry. H) Alignment process of LCEs during stamping. Reproduced with permission.[67] Copyright 2012, Institute of Physics
Publishing. All the rod-like drawings in the figures represent mesogens.

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along the loading direction, whereas multiaxial stretching
endows the LCEs with the multidirectional orientation[50]
(Figure 1B).
Different from tensile stress, compressive stress always indu-
ces the alignment of mesogens perpendicular to the stress.[51]
Compressive stress is achieved not only by uniaxial compression,
but also by the deswelling process.[52] Anisotropic deswelling
technology has been applied to obtain a planar orientation of
the director, which was utilized in preparing cholesteric
LCEs[53,54] (Figure 1C).
For LCE precursor solutions or thermoplastic LCEs, the shear
stress during their molding is an effective alignment induce-
ment. Researchers have proposed some shear stress-induced
alignment methods for LCEs. 4D printing is one typical method.
The shear stress[55–58] aligns the mesogens along the printing
path during the extrusion of viscous inks,[59] which is conducive
to achieving programmable orientation (Figure 1D). Therefore,
the deformation design of the LCEs can be built into the 3D print-
ing process simultaneously, enabling the fourth-dimensional
printing.[60] 4D printing provides a powerful solution for the com-
plex orientation in LCEs, such as gradient orientation[59] and
patterned orientation.[55,61] In addition, the shear stress has also
been used in the microfluidic alignment process (Figure 1E) to
prepare oriented micro-/nano-LCE droplets and shells,[62,63] as
well as in the fiber electrospinning[64,65] or drawing process
(Figure 1F)[27,66] to prepare oriented LCE fibers.
In some cases such as stamping,[67] crimping, and emboss-
ing,[68] the stress condition is complex and various types of
mechanical stresses are coupled to align LCEs (Figure 1G,H).
The predetermined patterns are easy to reproduce in the LCEs
by these technologies.
2.2. External Field-Induced Alignment
In addition to mechanical stress, the mesogens are also very
sensitive to the effect of external fields such as magnetic field,
Figure 2. Schematic diagrams of various external field-induced alignment methods. A) Aligning mesogens by magnetic field. Here, R represents
the intermediate bridge bond connecting the benzene rings, B represents the magnetic induction intensity, and n represents the director.
B) Aligning mesogens by electric field. Here, E represents the electric field intensity. C) Polarized light (365 nm) induces the reorientation of azobenzene
mesogens. Reproduced with permission.[6] Copyright 2019, John Wiley and Sons. All the rod-like drawings in the figures represent mesogens.
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electric field, light,[69] indicating that the alignment of LCEs
can be realized by the induction of external fields.
Most of the mesogens contain benzene ring structure, which
are strongly diamagnetic and tend to align along the direction
with the least magnetic flux.[70] Therefore, the mesogens are
always aligned along the direction of magnetic induction
intensity (Figure 2A).
Mesogens will deflect under an electric field. The deflection
direction is determined by the dielectric anisotropy of
LCEs, and the deflection magnitude is controlled by the electric
field intensity.[70] The long axes of positive (or negative) liquid
crystal molecules will rearrange along the direction parallel
(or perpendicular) to the electric field (Figure 2B). Because of
the layered structure of smectic liquid crystal materials, the
applied electric field can actuate the mesogen tilt in layers
through the electroclinic effect,[71–73] resulting in the expansion
or contraction of the layer thickness. Therefore, this effect can be
applied to the preparation[74] and electrostriction[7] of smectic
LCEs.
Photoalignment technology has also been widely used for the
preparation and actuation of LCEs. The previous review reported
the basic photoaligning materials and photoalignment mecha-
nisms.[75] Illumination causes the angular redistribution of pho-
tosensitive mesogens, and further makes them steadily align in
the direction perpendicular or parallel to the polarized light.[75,76]
The LCEs containing azobenzene mesogens are a typical class of
photoresponsive materials,[77,78] which are aligned by the induc-
tive effect of the light vector from 365 nm polarized light
(Figure 2C).
External fields can remotely induce and program the align-
ment of mesogens by adjusting the direction and intensity
distributions of the fields, enabling them popular in both the
preparation and actuation of LCEs. Note that, the external
field-induced alignment is more effective in realizing the radial
orientation of circular or annular LCEs than multiaxial stretching
alignment.[5,79]
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2.3. Surface Effect-Induced Alignment 3. Versatile Actuations for LCEs

When liquid crystal molecules are in contact with some special
surfaces, the mesogens will be induced to align under surface
effect. The surface effect originates from two aspects. On the
one hand, the intermolecular forces[80] between the mesogens
and the surface molecules (containing dipole moment) of
alignment layer materials (polyurethane,[81] polyimide,[82] epoxy
resin,[83] etc.) contribute to inducing alignment. On the other
hand, nanoscale or microscale channels (hereinafter referred
as microchannels) created on the surface of the alignment layers
are related to the alignment direction (Figure 3A). The alignment
capability of the microchannels on the mesogens is characterized
by anchoring strength.[83,84] When the mesogen director is
parallel to the direction of the microchannels, the anchoring
strength is largest[83] and the mesogens are in a stable state.
At present, the fabrication methods for microchannels are
mainly dependent on subtractive manufacturing such as
rubbing[22,29] (Figure 3B), photolithography[83,85] (Figure 3C),
and preparing anisotropic porous templates[86] (Figure 3D).
However, Yu and co-workers prepared highly oriented carbon
nanotube (CNT) sheets by chemical vapor deposition (additive
manufacturing) to align LCEs (Figure 3E), and improved their
mechanical strength (15.7 MPa higher than the pure LCEs in
the direction parallel to alignment) and electrical conductivity
(270 S cm1) simultaneously.[87]
Both the internal orientation structure (intrinsic factor) and exter-
nal stimuli (extrinsic factor) are indispensable to the deformation
actuations of LCEs. The programming design of the orientation
structure or/and external stimuli can create diverse deformation
modes such as expansion, bending, torsion, 2D-to-3D structural
transformation, and more complex deformations and motions. In
the early years, people focused on the programmability of the ori-
entation structure in LCEs to enrich deformation modes, but not
the external stimuli; in recent years, people have been interested
in the selectivity of external stimuli to diversify the deformation
modes, using the LCEs with simple orientation structure. This
review therefore summarizes the versatile actuations for LCEs
into two categories, based on programmable orientation structure
and selective external stimuli, respectively. Apparently, the simul-
taneous manipulation on both these two factors will considerably
expand the dimensions for the deformation actuations of LCEs,
but few investigations have been explored so far.
3.1. Versatile Actuations Based on Programmable Orientation
Structure
When LCEs are exposed to external stimuli, their deformation
directions are parallel to orientation directions. Therefore, the

Figure 3. Schematic diagrams of various surface effect-induced alignment methods. A) Principle of aligning LCEs by surface effect. B–E) Schematic
diagrams of different methods for preparing surface microchannels. B,C) shows the alignment templates prepared by rubbing and photolithography
on the surface of alignment layer materials, respectively. (B) Reproduced with permission.[127] Copyright 2012, Elsevier. (C) Reproduced with permis-
sion.[83] Copyright 2016, John Wiley and Sons. D) The alignment template from PVDF film with anisotropic pores. Reproduced with permission.[86]
Copyright 2017, John Wiley and Sons. E) The alignment template from oriented CNTs. Reproduced with permission.[87] Copyright 2012, John Wiley
and Sons.

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programmable patterning design of the orientation structure in
LCEs can realize various complex and abundant deformation
modes. The patterning precision of LCEs determines the control-
lability and precision of their deformation actuations. The orien-
tation structure in LCEs mainly includes two aspects of boundary
constraints and the mesogen orientation (orientation site, orien-
tation direction, and orientation degree). Therefore, the program-
mable orientation structure is accomplished currently through
two strategies: programming boundary constraints and program-
ming the mesogen orientation.
3.1.1. Programming Boundary Constraints
Through integrating the materials with different expansion coef-
ficients in an intralayer or interlayer manner, the constraint-
induced internal stress mismatch at the boundary will cause
deformation of the composite systems. For instance, the inter-
layer bonding between unoriented and oriented LCEs causes
bending deformation of LCE composites,[88] whereas the
double-layer LCE films with interlaced orientation directions
are prone to spiral deformation.[89] The introduction of patterned
constraints into LCEs is expected to achieve more versatile defor-
mation actuations. In this constraint-addition way, the bonding
performance of the boundary is the key issue to be solved.
Currently, the boundary bonding of LCEs mainly depends on
the polymerization of residual double bonds from acrylates[18]
or the crosslinking by disulfide bonds.[89]
In the other constraint-subtraction way, a simple cutting treat-
ment is adopted to create patterned free boundaries within ori-
ented LCEs, so as to complete predesigned deformation. Zeng
and co-workers realized the 2D-to-3D deformation of LCE films
on the basis of kirigami design, which was utilized to design a
rolling soft robot with multiple optomechanical petals.[90] In
comparison with the relatively high technology and equipment
requirements to program the mesogen orientation, program-
ming boundary constraints is a simple and potential technology
to realize versatile actuations for LCEs, but it has not attracted
enough attention at present.
3.1.2. Programming the Mesogen Orientation
Programming the mesogen orientation is the most effective and
popular way to achieve versatile actuations for LCEs. This way
drives the stimuli–responses by the heterogeneity in the local
orientation, but not the heterogeneity in material composition.
We summarize four common alignment methods for patterned
orientation from Table 1, as photolithography alignment,
embossing alignment, template-induced alignment, and 4D
Table 2. Alignment methods for programming the mesogen orientation and their deformation controllability.
Alignment Method Patterning precision Programmability of the mesogen orientation
Orientation site
p [50,92,93]
Photolithography alignment 10 μm
p [67,68,94]
Embossing alignment 1 mm [67,68,94]
p[83,95,98,135]
Template-induced alignment 1 μm[83,96,98]
p[55,58,59,100,130]
4D printing alignment 100 μm[55,59,61,101]
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printing alignment. These methods are shown in Table 2 and
compared in terms of patterning precision, programmability,
and deformation controllability.
Photolithography alignment is suitable for the LCEs prepared
by photocrosslinking. In this method, the weakly crosslinked liq-
uid crystal polymer in the aligned state is covered by a patterned
photomask. The residual double bonds in the light-transmitting
areas of the photomask are crosslinked by UV light to finish the
curing procedure, thereby retaining the mesogen orientation. By
contrast, the mesogens in the light-shielding areas are unor-
iented after the external force is unloaded. As a result, the pho-
tomask pattern is reproduced within the prepared LCEs by the
orientation distribution.[91] Chen and co-workers prepared the
LCEs with patterned orientation by this method (Figure 4A)
and realized their crawling motion under light scanning
(Figure 4B).[92] Moreover, the photolithography operation can
also be carried out first before the alignment process of the
weakly crosslinked liquid crystal polymers (Figure 1B). If so,
the uncrosslinked part in the light-shielding areas can be aligned
and crosslinked subsequently to obtain LCEs with patterned
orientation.[50,93]
The essence of embossing alignment is to align the mesogens
at the edge of the embossed pattern by mechanical stamping
(Figure 1H). One LCE film is sandwiched between female and
male molds to replicate the mold patterns. Cai et al. synthesized
a LCE containing dynamic disulfide bonds, which would cleave at
180  C to generate free radicals. These free radicals existed for
several hours at room temperature because of chain transfer
reactions. Therefore, this LCE can be embossed and aligned at
room temperature after high-temperature treatment. After main-
taining the alignment of the mesogens long enough, the liquid
crystal network is cured again to fix the mesogen orientation.
This kind of LCE with special chemical structure can easily pro-
gram the orientation pattern by the combination of female and
male molds, so that the LCE possesses the shape memory func-
tion for the mold patterns (Figure 4C,D).[94]
In template-induced alignment, the mesogen orientation with
topological defects can be obtained through programming the
microchannel pattern of the template. The alignment principle
is that the mesogens match the size of microchannels to form
the largest anchoring strength with the surface through director
rearrangement. In experiments, the microchannel precision of
the template attains the order of 1 μm,[83] so high-precision
orientation patterns can be designed by the template-induced
alignment method. Yang and co-workers prepared the oriented
LCE film with 5
5 array of topological defects, which can realize
a 2D-to-3D folding transformation,[95] and lift the load up to 734
times its own weight by conical deformation (Figure 4E).[83] The
Deformation controllability Illustration
Orientation direction Orientation degree



Figure 4A,B



Figure 4C,D
p[83,95,98,135] p[83,98]

Figure 4E
p [55,59,100,130] p[58,59,100,130] p [55,100,130]
Figure 4F,G,H
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Figure 4. Versatile deformation actuations of LCEs based on programmable mesogen orientation. A) Schematic diagram of a patterned LCE film pre-
pared by photolithography alignment. B) Crawling motion of the LCE prepared by the method of A) under infrared light scanning. A,B) Reproduced with
permission.[92] Copyright 2019, American Chemical Society. C) Schematic diagram of programming disulfide LCE films by embossing alignment at room
temperature. D) Reversible and thermal actuation of the patterned disulfide LCE film. C,D) Reproduced with permission.[94] Copyright 2019, Royal Society
of Chemistry. E) Fabricating conical LCE actuators by template-induced alignment. (i) Microchannel pattern for aligning the mesogen orientation with
“þ1” topological defects; (ii) optical image of a LCE sheet containing 5
5 array of “þ1” defects at room temperature; (iii) lifting 6.83 g load by conical
LCE actuators. Reproduced with permission.[83] Copyright 2016, John Wiley and Sons. F) Utilizing 4D printing alignment to realize multiple deformation
modes of LCEs. Reproduced with permission.[55] Copyright 2017, American Chemical Society. G) Programming the orientation degree of 4D-printed LCEs
based on a temperature gradient. Reproduced with permission.[59] Copyright 2019, American Chemical Society. H) Programming the orientation degree
of 4D-printed LCEs based on a gradient of print speed. Reproduced with permission.[100] Copyright 2020, American Chemical Society.

deformation characteristics of the LCEs aligned by the micro- actuated just by designing the microchannel patterns.[96,97]
channels depend on the strength and pattern of the topological By theoretical analysis and numerical calculation, Yang and
defects, so rich and diversified deformation modes can be co-workers and White and co-workers designed special

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microchannel topology patterns to achieve the on-demand 3D
deformation of initially flat LCE films.[98,99]
4D printing alignment has excellent pattern programmability
due to the local control of both orientation direction and orien-
tation degree. The orientation direction in LCEs is programmed
along the printing path. Ware and co-workers prepared various
patterned LCEs by controlling the 4D printing path, and achieved
conical, helical, and contractive deformation actuations
(Figure 4F).[55] The orientation degree of 4D printed LCEs is pro-
grammed by printing temperature or printing speed. Zhao and
co-workers set a temperature gradient to print grid-patterned
LCEs with controllable gradient orientation, and completed
the shape transformation from a 2D porous plane to a 3D porous
cylinder (Figure 4G).[59] Ren and co-workers varied the printing
speed to encode local orientation degree into a linear LCE, and
realized snake-like curling deformation (Figure 4H).[100] In the
fields of soft devices and soft robots, thermally or electrically con-
trolled LCE hinges were prepared on the basis of 4D printing,
and further integrated in the applications of grippers, foldable
structures, and walking robots.[1,101,102]
To sum up, the aforementioned four methods can all access
the patterned orientation in LCEs. Photolithography alignment
and embossing alignment show the relatively weak deformation
controllability due to the absent programmability for orientation
direction. By contrast, template-induced alignment and 4D print-
ing alignment show the strong deformation controllability for
LCEs. In terms of the patterning precision, template-induced
alignment provides a high control precision of 1 μm for the
mesogen orientation, but is limited to fabricate LCE films with
the thickness less than 100 μm; whereas 4D printing alignment
has a low control precision of 100 μm, but the resultant LCEs
are unrestricted in size. Therefore, how to precisely control the
patterned orientation in LCEs with arbitrary geometric dimen-
sions is a big difficulty in designing functional LCEs.
3.2. Versatile Actuations Based on Selective External Stimuli
As the triggering condition of deformation in LCEs, external
stimuli such as light and heat can be selectively applied in terms
of their sources and sites, which can effectively control the local
deformation of LCEs and produce various deformation and
motion modes. As the application of external stimuli is easily pro-
grammed and controlled by microcomputers or other control
devices (the presence or absence of stimulus at different sites
of LCEs can be represented by binary numbers), utilizing
selective stimuli to actuate LCEs is conducive to the digitalization
of controlling the local deformation of LCEs. The actuation
methods by selective external stimuli and their deformation
controllability are shown in Table 3.
Table 3. Actuation methods by selective external stimuli and their deformation controllability.
Selection of stimulus objects Stimulus forms
Stimulus sources Switching
Stimulus sites Gradient
Scanning Crawling[14,17,92,109] and rotating,[109,110] etc.
Programming Programmable deformation
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3.2.1. Selectivity of Stimulus Sources
The multimaterial integrated design of LCEs with different
stimuli–responses can endow the composite LCEs with multisti-
muli responses.[103,104] By switching different stimulus sources,
switchable deformation modes of LCEs can be achieved.
Common switching operations occur between light and heat,
between different types of light sources, or between thermal
stimuli at different temperatures. Yang and co-workers fabri-
cated the double-layer LCE strip composed of one LCE layer con-
taining azobenzene mesogens and the other LCE layer with
photothermal-response characteristics. The former layer can
respond to UV light through the cis–trans isomerization reaction
of the azobenzene mesogens, whereas the latter layer can
respond to NIR light due to the photothermal-induced deforma-
tion. Therefore, when the stimulus source is switched, this
double-layer LCE exhibits opposite spiral curling deformation
(Figure 5A).[103] For the LCE films containing azobenzene meso-
gens, the polarization direction of linearly polarized light can be
switched to control their bending direction.[105] When LCEs with
different nematic-to-isotropic transition temperatures are inte-
grated into the same device, the local deformation can be actu-
ated sequentially by switching the actuation temperature.[1,56]
3.2.2. Selectivity of Stimulus Sites
Selective stimuli toward the specific sites of LCEs can effectively
control their local deformation to complete specified motions or
functions. This review divides the selectivity of stimulus sites
into three forms, namely gradient, scanning, and programming
stimuli.
Gradient stimulus controls the gradient distribution of stim-
ulus intensity at different sites of LCEs, which can easily cause
the bending deformation of LCEs.[106] Light is a kind of noncon-
tact and easy-to-manipulate stimulus source, so gradient optical
stimulus or photothermal stimulus has been the most widely
used stimulus form. Yu et al. used attenuated light with an inten-
sity gradient to induce the deformation of the LCE microtubes
from a cylinder to a cone, resulting in a capillary force that drives
a fluid slug toward the thin end. They also demonstrated the
back-and-forth motion of the fluid slug in the microtubes by
alternating the gradient direction of the light intensity
(Figure 5B).[107] Hayward et al. deposited gold plasmonic
nanoparticles with photothermal-response characteristics on
the surface of the LCE fibers. Using waveguided light to induce
thermal gradient, they actuated the bending deformation of the
LCE fibers. The bending angle increased with the power of wave-
guided light.[108]
Deformation modes Deformation controllability Illustration
Switchable deformation
Figure 5A
Bending , [106,108,136]
etc.
Figure 5B

Figure 5C
p [8,9,15]
Figure 5D
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Figure 5. Versatile deformation actuations of LCEs based on selective external stimuli. A) Actuating left and right spiral curling of a double-layer LCE strip
by switching light sources. (i) Schematic diagram; (ii) optical images. Reproduced with permission.[103] Copyright 2018, Taylor & Francis. B) LCE micro-
tubule actuators in response to attenuated light with an intensity gradient. (i) Schematic diagram of photoinduced deformation of LCE microtubes; (ii)
Lateral photographs of the back and forth motion of a silicone oil slug in a tubular microactuator actuated by alternating the gradient direction of light
intensity. Reproduced with permission.[107] Copyright 2016, Springer Nature. C) Rotation of a LCE disk actuated by structured light scanning stimulus
(green arrow: direction of the traveling wave; black or white arrow: rotation direction of the LCE disk; green coverage area: light scanning position; dashed
and red lines: reference lines before and after driving). (i) Schematic diagram; (ii) optical images. Reproduced with permission.[109] Copyright 2016,
Springer Nature. D) LCE-based soft tubular actuators with programmable on–off control. (i–iv) Preparation process of the soft tubular actuators;
(v) several actuation modes of the soft tubular actuators controlled by different power-on and power-off combinations, and the insets show the
power-on and power-off states of the resistance wires. Reproduced with permission.[8] Copyright 2019, American Association for the Advancement
of Science.

Scanning stimulus is to actuate LCEs through periodic site
stimulus. The stimulus characteristic at each site is dynamic
and periodic, and the scanning direction determines the motion
direction of LCEs. Utilizing the linear scanning light, the creep-
ing motion of LCEs was realized in crawler-like soft
robots.[14,17,92,109] Utilizing the circular scanning light, the
directional rotation of LCEs was realized, to manufacture
light-controlled or photothermally controlled micromotors
(Figure 5C).[109,110] Not only stimulus sources but also LCEs
can act as the actively moving ones. Inhomogeneous deformation
generated by the local stimulus in the LCEs will induce the dis-
placement of the centroid of a LCE device, which leads to the

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change of stimulus sites and thus persistently actuates the
motion of the LCE device. Several examples have adopted
this stimulus form successfully, such as the LCE wheels and
helical ribbons designed by Zhao and co-workers[4] the LCE
light-fueled cantilever oscillators designed by White and co-work-
ers,[34,111] and the LCE electric locomotives designed by Yang and
co-workers.[112]
Programming stimulus can achieve versatile actuations of
LCEs by digital control of both stimulus sites and the stimulus
intensity, thereby having a huge advantage in complex actuators
and soft robots. To digitize the stimulus conditions, researchers
often use electric potential to control the stimulus sources. For
instance, when patterned heating wires are integrated into ther-
motropic LCE layers, rich and diverse deformation modes are
demonstrated by electrifying the heating wires selectively
(Figure 5D). The deformation degree of LCEs can also be readily
controlled by the design of parameters such as the applied
voltage, power-on time, and material sizes.[8,9,15,113,114] When
LCEs are doped with photothermal-responsive nanoparticles
such as CNTs[16,115,116] or polydopamine,[28,117] the doped
sites will respond to the photothermal stimulus. Therefore, a
wealth of deformation modes of LCEs can be actuated
through programming the doped sites.[116,118] Ji and co-workers
pasted photothermal-responsive LCE strips on other soft materi-
als to achieve similar local thermal actuation, which provides a
simple method for pattern programming of photothermal
stimulus.[117]
By means of selective external stimuli, versatile deformation
actuations of LCEs can be fully exploited without designing com-
plex orientation structure. Four common actuation methods
based on selective external stimuli and their deformation control-
lability are shown in Table 3. The method of switching stimulus
sources is mainly applicable to multiresponse material integra-
tion systems, and is limited by the number of switchable defor-
mation modes. Gradient and scanning stimuli also produce only
a few specific deformation modes, such as bending, crawling, or
rotating. In contrast, programming stimulus can greatly expand
the deformation space for LCEs and increase their motion free-
dom, which is expected to realize the complex functions or
motions of soft devices and soft robots. Except programming
the orientation structure of LCEs, selective external stimuli, serv-
ing as the other effective way to achieve versatile actuations of
LCEs, has drawn more attention in recent years.
4. Conclusions
Owing to the rapid development of soft devices and soft robots,
LCEs, serving as a class of typical intelligent soft materials, have
attracted more and more attention. In this review, we summarize
the research progress of varied alignment methods and versatile
actuations for LCEs in recent years. This review aims to help
people to design and prepare LCE materials with programmable
orientation structure and excellent actuation characteristics, and
expand their applications in related fields. To meet the require-
ments of practical applications, developing versatile, precise, and
fast-responsive deformation actuations for LCEs is the central
challenge in the future. The corresponding key technologies
are envisioned as follows.
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4.1. Versatility
The rich and reversible deformation and motion modes of LCEs
are the typical characteristics that distinguish them from other
intelligent soft materials such as shape memory polymers, gels,
and liquid metals. Through material and structural designs and
innovations in actuation technologies, it is expected to achieve
more versatile deformation actuations for LCEs. 1) Material
and structural designs: Through integrating heterogeneous
materials and structures with different properties at multiple spa-
tial scales, the mechanical properties[87,117,119,120] and stimuli–
responsive performances[2,11,121–125] of LCE composites can be
tuned to a large extent, so as to enrich the deformation modes
of LCEs. The common multiscale integration designs include
adding nanoparticles (nanoscale), designing interpenetrating
polymer networks or phase separation structure (mesoscale),
patterning integration for multimaterials by 4D printing (micro-
scale), and intralayer or interlayer bonding of multimaterials
(macroscale). 2) Innovations in actuation technologies: internal
orientation structure and external stimuli are the intrinsic and
extrinsic factors to realize deformation actuations for LCEs,
respectively. To accomplish versatile actuations, the former
has been widely studied in terms of programming design, espe-
cially based on template-induced alignment and 4D printing
alignment. However, the latter is still relatively less studied
and has a large research space. Programming external stimuli
through microcontroller-based digital control is a potential actu-
ation technology for the versatile deformation of LCEs. In the
future, the simultaneous manipulation on both these two factors
will considerably expand the dimensions for the deformation
actuation of LCEs.
4.2. Precision
The programmed orientation structure of LCEs is realized by the
design of patterned orientation distribution. Therefore, the pre-
cision of orientation patterns is the decisive factor for actuating
the precise deformation of LCEs. Just as liquid crystal displays
can show excellent display performance with high resolutions,
LCEs may also exhibit more precise and controllable deformation
actuations with higher orientation programming precision. In
the existing reports, both template-induced alignment and 4D
printing alignment have shown strong programmability. The for-
mer shows the programming precision of 1 μm dependent on
the microchannel size on the template,[83,96,98] whereas the latter
shows the programming precision of 100 μm dependent on the
size of printer nozzles.[55,59,61,101] These sizes are still 3–6 orders
of magnitude larger than the size of liquid crystal molecules,
indicating there is still room for further improvement in pro-
gramming precision of domain orientations. The development
of high-precision programmable alignment methods is a prereq-
uisite for realizing the precise actuation of LCEs.
4.3. Responsiveness
Due to the advantages of thermal stimulus such as strong pene-
trability and large actuated deformation, the current LCE-based
applications mostly adopt direct thermal, photothermal, or
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electrothermal stimuli. But there is a serious problem of
slow response speed in the form of thermal stimulus. Cai and
co-workers reported that LCEs take 30 s for the full thermal-
induced contraction, but 4 min for the full recovery to the initial
state.[8] The slow response problem has significantly limited the
development of LCEs for practical applications. Direct field stim-
uli such as light, electric field, and magnetic field may produce
fast-responsive and reversible deformation actuations for LCEs
and promote their practical process.
Acknowledgements
This project was supported by the National Natural Science Foundation
of China (11702207).
Conflict of Interest
The authors declare no conflict of interest.
Keywords
actuations, alignments, liquid crystal elastomers, orientation,
programmability
Received: April 12, 2021
Revised: September 25, 2021
Published online: November 7, 2021
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Jiayou Zhao obtained his bachelor’s degree, in 2019, majoring in mechatronics engineering, from North
China Electric Power University. He joined Prof. Jian Hu’s research group, in 2019 as a postgraduate
student at State Key Laboratory for Strength and Vibration of Mechanical Structures, School of Aerospace
Engineering, Xi’an Jiaotong University. He is now working on LCE actuators.

Limei Zhang obtained her bachelor’s degree, in 2014, majoring in chemistry from Changzhi University.
She has been a Ph.D. student at State Key Laboratory for Strength and Vibration of Mechanical
Structures, School of Aerospace Engineering, Xi’an Jiaotong University. She is now working on the
preparation of soft materials and their applications in flexible electronics.

Jian Hu is a professor at School of Aerospace Engineering in Xi’an Jiaotong University (XJTU). He

graduated in chemical engineering and technology from Zhejiang University, in 2006, and obtained his
master’s degree in 2008. He received his doctor’s degree from Hokkaido University, Japan, in 2012. He
worked as a postdoctor in Hokkaido University for 3 years. In 2016, he was recruited as a professor at
School of Aerospace Engineering in XJTU. He focuses on the study of soft materials and mechanics of
soft materials, including synthesis of polymer soft materials, structural design, mechanics and
multifunction, and intelligent soft material devices.

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