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Danny Goldman as Brainy Smurf (voice)
Amber May as Kami
Kan Tokumaru as David Ryan (voice)
Allison Janney as Madge Nelson (voice)
Yuichi Nakamura as Nemesis 009/Graviton
Brigitte Virtudes as Tyrannia
Joshua Olsthoorn as (voice)
Anthony Quayle as Narrator (voice)
Luis Tosar as Xavier
Hikaru Midorikawa as Bakuryuu TopGaler (voice)
Liam O'Brien as Hiroim (voice)
Rimi Nishimoto as Rimi Ushigome
Kimiko Glenn as Kiff
Luis Posada as Mr. Money (voice)
Chiwa Saito as Lexie Willow Carter
Rikako Aikawa as Cleffy (voice)
Alexandra Essoe as Katie
Kaori Fukuhara as Astrea (voice)
Tom Milligan as Edred / Dimitri
Jim Broadbent as Ernest Briggs (voice)
Miu Yuzuhara as Haruki Azuma

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