• 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
Ending Movie: Les Acteurs Incroyable
Last Battle Intro Movie: Les Acteurs Incroyable
Opening Movie: Riddle Of The Incan Empire!