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When you complete Arcade mode with a character you will be able to unlock the character's model in the Archive menu.
Unlock Chrono's Model:
Complete Arcade mode with Chrono.
Unlock Fate's Model:
Complete Arcade mode with Fate.
Unlock Hayate's Model:
Complete Arcade mode with Hayate.
Unlock Material-D's Model:
Complete Arcade mode with Material-D.
Unlock Material-L's Model:
Complete Arcade mode with Material-L.
Unlock Material-S's Model:
Complete Arcade mode with Material-S.
Unlock Nanoha's Model:
Complete Arcade mode with Nanoha.
Unlock Reinforce's Model:
Complete Arcade mode with Reinforce.
Unlock Shamal's Model:
Complete Arcade mode with Shamal.
Unlock Signum's Model:
Complete Arcade mode with Signum.
Unlock Unison Reinforce's Model:
Complete Arcade mode with ALL the characters.
Unlock Vita's Model:
Complete Arcade mode with Vita.
Unlock Zafira's Model:
Complete Arcade mode with Zafira.
When you complete the following tasks the corresponding hidden character will become availalbe in Player VS. COM mode.
Unlock Material S (Starlight Destroyer):
Complete Story mode in vertical lane as Nanoha Vita and Zafila.
Unlock Material L (Dark Hayate):
Complete Story mode in vertical lane as Hayate Shamal and Reinforce.
Unlock Material M (Dark Fate):
Complete Story mode in vertical lane as Fate Signum and Chrono.