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When you complete the indicated task the corresponding character will become unlocked.
Roronoa Zoro:
Complete Episode 1, 'Shells Town'.
Nami:
Complete Episode 2, 'Orange Town'.
Usopp:
Complete Episode 3, 'Syrup Village'.
Sanji:
Complete Episode 4, 'Baratie'.
Portgas D. Ace:
Complete the main storyline.
Travel from Loguetown to Shells Town, then to Windmill Village, then to Baratie, and finally to Loguetown. When you have done this a new island named 'Aokiji' will appear.