Successfully complete Trial 29 to unlock Android Rachel.
Play as Charles The Third
Successfully complete the second level of Story mode to unlock Charles The Third.
Play as Devil Buster Dante
Successfully complete the first level of Story mode (all four chapters) to unlock Devil Buster Dante.
Play as Director Blue
Successfully complete Trial 1 to unlock Director Blue.
Play as Fighter Bianky and Friends
Successfully complete Trial 13 to unlock Fighter Bianky and Friends.
Play as Gran Bruce
Successfully complete Trial 35 to unlock Gran Bruce.
Play as Heroine Silvia
Successfully complete Trial 37 to unlock Heroine Silvia.
Play as Hulk Davidson
Successfully complete Trial 14 to unlock Hulk Davidson.
Play as Manager Jet
Successfully complete Trial 19 to unlock Manager Jet.
Play as Movie Fan Joe
Successfully complete Trial 5 to unlock Movie Fan Joe.
Play as Stylish Alastor
Successfully complete Trial 34 to unlock Stylish Alastor.
Play as Young Blue Jr.
Successfully complete Trial 24 to unlock Young Blue Jr.
Play as Young Captain Blue
Successfully complete Trial 40 to unlock Young Captain Blue.
Alternate costumes
Successfully complete all 40 Trial mode missions to unlock alternate costumes for all characters. Highlight a character at the chracter selection screen, then press Square to change their costume.
Special Story mode stages
Collect the sixteen puzzle pieces in each stage in Story mode to unlock Special Story mode stages.
Art gallery
Collect all sixteen puzzle pieces in each Special stage in Story mode to unlock the Art gallery.
Movies
Successfully complete the indicated Story mode chapter to unlock the corresponding movie:
Atlantis: Four Adventures Of The Sea: Gulliver's Battles
Atlantis: Four Adventures Of The Sea Special Edition: V-Puzzle 6
Boss*Boss*Bang*Bang: All previous chapters except The Hidden Hideout
Captain Blue Begins: Viewtiful Cartoon World
Captain Blue Begins Special Edition: V-Puzzle 3
Gulliver's Battles: Truth Of The Black Film
Gulliver's Battles Special Edition: V-Puzzle 5
Les Acteurs Incroyable: Atlantis: Four Adventures Of The Sea
Red Hot Rumble: Boss*Boss*Bang*Bang
Riddle Of The Incan Empire! Special Edition: V-Puzzle 1
The Hidden Hideout: Any chapter with Charles The Third, Hulk Davidson, and Gran Bruce
Truth Of The Black Film: Captain Blue Begins
Truth Of The Black Film Special Edition: V-Puzzle 4
Viewtiful Cartoon World: Riddle Of The Incan Empire!
Viewtiful Cartoon World Special Edition: V-Puzzle 2