Chris Sanders as Stitch, the main protagonist of the film.
Jessica Chastain as
Angel, Stitch's love interest. Hayden Panettiere as
Yuna, Stitch's tomboyish friend. David Ogden Stiers as Jumba Jookiba, an evil genius scientist, the one who created Stitch, and the other 625 Experiments. He is assigned by the Galactic Council to watch over Stitch, and lives with Yuna and Obaa. He is more friendly in this series than the original, and has less of a penchant for evil.
Bill Hader as Agent Pleakley, Jumba's sidekick.
Michael Caine as
Flint, British spy alien who is Stitch's cousin. Leslie Mann as
Sarah, Hungarian spy alien who is Stitch's cousin and Angel's half sister. Kelsey Grammer as Professor Waltom, a corrupt British scientist alien and is main anatogonist.
Thomas Kretschmann as Doctor Bundapp, a German-accented alien who is Jumba's former creation and Waltom's assistant. He's also Flint's arch-nemesis.
Michael Bell as Vultor, Waltom's pet vulture with a pistol on her right wing and a cybernetic right eye that forms a video camera and laser gun.
Dave Wittenberg as Slickfoot, Waltom's sleazy lawyer. His voice was similiar to Tony Jay.
Jeffrey Garcia and Davi Vieira as Elmo and Eggo, Doctor Bundapp's bullies with Spanish accent.
Brad Garrett as Hago, Doctor Bundapp's lieutenant with Cockney accent.