Hiro Shimono (JP)/Bill Hader (EN) as Deine Astray

Rina Sato (both JP/EN) as Kaori Mochizuki

Mark Berry (CD-I Ganon) or Peter Cullen (Optimus Prime) as Backlife
Yūichi Nakamura (JP, the one who voices Yoshiki Kishinuma)/Charles Lee Ray's VA (EN) as
Dunkman
Harry S. Robins (EN) as Aleinekov, Orpheus, Colt, Telestar, and Dr. Wolfgang
Koumei Satou himself (JP)/Tony Todd (EN) as Eltagon Eupendou and Omnize
Tomokazu Sugita (JP)/Peter Berkrot (EN) as Mephes
Jūn Osuka (JP) as Palze Orville
Eri Kitamura (JP)/Sarah Williams (EN) as Polika Elteen
Miyuki Sawashiro (JP)/Merle Dandridge (EN) as Siline Casty
Tetsuya Kakihara (both JP and? EN; said VA has apparently learned some English)/ Lennon
Adams (EN) as Elba Astray
Ayano Yamamoto (JP)/Jennifer Tilly (EN) as Tena Hive
Daisuke Matsuo (JP)/John Patrick Lowrie (EN) as Dolce Notein, Paltmar Tehind, and Opponity
Tehind
Asami Imai (JP)/Lennon Adams (EN) as Alphobia
Yuka/Yuuka Nanri (JP) as Valenia Tastonel

The Subsequence bonus episode:

Asami Imai (JP) as Kiyomi
Hiro Shimono (JP) as Kishi
TBA as the rest of the students

The Uprising, Aftermath, and Conclusion game ideas:

Jūn Osuka, Tomokazu Sugita, and Yūichi Nakamura (JP)/Peter Berkrot, Lennon Adams, and
Charlie Ray's VA (EN) as Ulmseean Metroprotectors, Ulmseean Soldiers (Palze's type) and
Ulmseean Elite Soldiers (Mephes' type)
Yūichi Nakamura, Tomokazu Sugita, Tetsuya Kakihara, Daisuke Matsuo, and Hiro Shimono
(JP)/ Charlie Ray's VA, Lennon Adams, Tony Todd, and Bill Hader (EN) as the male
Darlestorians and Citizens
Eri Kitamura, Seiko Yoshida, Asami Imai, Satomi Arai, and Miyuki Sawashiro (JP)/ Sarah
Williams, Merle Dandridge, and Jennifer Tilly (EN) as the female Darlestorians and female
Citizens
Taira Kikumoto (JP)/ Lennon Adams (EN) as Dr. Albertson, Ulmzeer of Ulmseea
Satomi Arai (JP)/ Sarah Williams (EN) as Emilia Casty
Asami Imai (JP)/ Lennon Adams (EN) as the Ulmseean Overwatch