The 59-year-old actor will play Titanium Rex, the leader of a worn-down superhero group desperate to remain relevant, reported Entertainment Weekly.
The 13-episode stop-motion series will air on Crackle, Sony's online streaming service.
Other cast members include Keegan-Michael Key, Jillian Bell and Seth Green.
Cranston will executive produce alongside Green and Robot Chicken's Matthew Senreich, who is writing the project with Zeb Wells.
Crackle also announced that Dennis Quaid will star in the service's new 10-part drama "The Art of More", which follows the "surprisingly cutthroat world of premium auction houses".
"Supermansion" and "The Art of More" will premiere on Crackle later this year.
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