Cast
- Freddie Highmore as Toby Tenma / Astro Boy. Toby is Dr. Tenma's son who is tragically killed in the Introduction. Astro is a robotic replica of Toby built in his image and with his memories. Rejected by his father, Astro is trying to find his place in the world. While in the manga, he is run by a technology called "kokoro" (Japanese for "heart"), Astro runs on Blue Core energy in the film.
- Nicolas Cage as Dr. Bill Tenma, Toby's father, creator of Astro, and head of Metro City's Ministry of Science
- Kristen Bell as Cora, a tomboy kid who lives on the Surface and is Astro's love interest.
- Bill Nighy as Professor Simon Elefun, Dr. Tenma's friend & associate and as Robotsky of the Robot Revolutionary Front.
- Donald Sutherland as President Stone, the ruthless President of Metro City who is running for re-election. He serves as the main antagonist of the film.
- Samuel L. Jackson as ZOG, a 100-year-old construction robot brought back to life by Astro's blue-core energy
- Nathan Lane as Hamegg, a surface-dweller who repairs machines and then uses them in his fighting tournament
- Matt Lucas as Sparx, the leader of the Robot Revolutionary Front.
- David Bowers as Mike the Fridge, a talking refrigerator and third member of the Robot Revolutionary Front
- Charlize Theron as "Our Friends" Narrator, of an educational video seen at the film's beginning
- Eugene Levy as Orrin, the robotic servant of the Tenma household
- Moisés Arias as Zane, a surface-dwelling child
- Alan Tudyk as Mr. Squeegee, a cleaning robot
- David Alan Grier as Mr. Squirt, a cleaning robot
- Madeline Carroll as Widget, twin of Sludge
- Sterling Beaumon as Sludge, the twin of Widget
- Dee Bradley Baker as Trashcan, a dog-like robot who serves as a literal bin
- Elle Fanning as Grace (cameo only) a girl from Hamegg's house who kicks President Stone in the shins
- Ryan Stiles as Mr. Mustachio, Toby's teacher.
- Newell Alexander as General Heckler, President Stone's head of military.
- Victor Bonavida as Sam, a teen from Hamegg's house
- Tony Matthews as Cora's father
- Bob Logan as Stinger One, President Stone's minion pilot who wants to capture Astro
- Ryan Ochoa as Rick, another boy from Hamegg's house
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