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These evil characters are unlocked by playing through 'Tournament' mode as the indicated character.
Unlock Mr. Crocker:
Beat 'Tournament' mode as Timmy.
Unlock Professor Calamitous:
Beat 'Tournament' mode as Jimmy.
Unlock Vlad plasmius:
Beat 'Tournament' mode as Danny.
Unlock Plankton:
Beat 'Tournament' mode as Spongebob.