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Complete Shipreck City in Story mode.

At the start menu press Triangle, Square, Triangle, Circle, Circle, Square and you'll block all the attacks.

Successfully complete the first mission at the Prison Fortress.

Successfully complete the indicated task to unlock the corresponding character:

Ammand The Corsair: Successfully complete the Pirate Poker sub-mission in the Shipwreck City level.
Black Bart: Successfully complete the Combat Challenge in the Maelstrom level.
Bootstrap Bill Turner: Successfully complete the Defeat Enemies sub-mission in the Prison Fortress level.
Cannon Arm: Successfully complete the Combat Challenge in the Pearl vs. Kraken level.
Capitain Chevalle: Successfully complete the Port Royal level.
Captain Barbossa: Successfully complete the Shipwreck City level.
Captain Elizabeth Swann: Successfully complete the Combo Challenge in the Davy Jones Locker level.
Captain Jack Sparrow: Successfully complete the Prison Fortress level.
Captain Sao Feng: Successfully complete the Singapore level.
Captain Teauge: Successfully complete the Combat Challenge in the Prison Fortress level.
Cotton: Successfully complete the Rescue sub-mission in the Isla de Pelegostos level.
Davy Jones: Successfully complete Pearl vs. Dutchman level.
Elizabeth Swann: Successfully complete the Tortuga level.
Gentlemen Jocard: Successfully complete the Davy Jones Locker level.
Gibbs: Successfully complete the Combat Challenge in the Port Royal level.
Governor Swann: Successfully complete the Combat Challenge in the Pearl vs. Dutchman level.
James Norrington: Successfully complete the Combat Challenge in the Tortuga level.
Lian: Successfully complete the Combat Challenge in the Singapore level.
Lord Cuttler Beckett: Successfully complete the Maelstrom level.
Mercer: Successfully complete the Hit-Combo sub-mission in the Singapore level.
Mistress Ching: Successfully complete the Jackanism in the Tortuga level.
Mordillah: Successfully complete the Combo Challenge in the Prison Fortress level.
Pintel: Successfully complete the Isla Cruces level.
Ragetti: Successfully complete the Combat Challenge in the Isla Cruces level.
Sri Sumba Jee: Successfully complete the Combat Challenge in the Shipwreck City level.
Tai Huang: Successfully complete the Sea Battle level.
Tia Dalma: Successfully complete the Missing Person sub-mission in the Port Royal level.
Villanueva: Successfully complete the Combo Challenge in the Tortuga level.
Will Turner: Successfully complete the Isla de Pelegostos level.

Go to a Loot Challenge in Multi-player mode. Have both players kill enemies but only have one person collect the loot.