In Villainous: Bigger and Badder, each player takes control of one of three Disney characters, each one a villain in a different Disney movie, specifically Syndrome (The Incredibles), Lotso (Toy Story 3), and Madam Mim (The Sword in the Stone).

Villainous: Bigger and Badder is playable on its own, and its characters can also face off against those in the other Disney Villainous games.