| Character | How to unlock
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|---|
| A.I.M. Agent | Complete level 10 "That Sinking Feeling".
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| Abomination | Complete level 4 "Rock up at the Lock up".
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| Agent Coulson | Complete the "Tabloid Tidy UP" bonus level.
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| Aldrich Killian | Complete level 5 "Rebooted, Resuited".
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| Ant-Man | Collect the Ant-Man token in the Industrial District.
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| Archangel | Collect the Archangel token south of the X-Mansion (south of giant billboard).
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| Arnim Zola | Complete level 6 "Red Head Detention".
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| Beast | Complete level 8 "Juggernauts and Crosses".
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| Beetle | Collect the Beetle token at one block east of the Central Park lake.
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| Black Cat | Collect the Black Cat token the cat pet shop directly under Lady Liberty on the map; requires Spider-Man.
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| Black Widow | Complete level 3 "Exploratory Laboratory".
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| Blob | Collect the Blob token after completion of the "Put Up Your Dukes" bonus level.
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| Captain America | Complete level 2 "Times Square Off".
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| Captain America (Comics) | Complete "The Brick Apple" bonus level.
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| Captain Britain | Complete the "The Brick Apple" bonus level.
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| Colossus | Collect the Colossus token at the front right courtyard of the X-Mansion.
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| Cyclops | Complete level 8 "Juggernauts and Crosses".
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| Damage Control | Collect the Damage Control token by putting out fires on the S.H.I.E.L.D. Helicarrier deck with the water gun.
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| Deadpool | Collect all Deadpool Red Bricks.
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| Doc Ock | Complete level 2 "Times Square Off".
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| Doc Ock (Ultimate) | Complete the "Tabloid Tidy UP" bonus level.
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| Doombot | Complete level 9 "Doctor in the House".
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| Drax the Destroyer | Complete Story mode, then complete 3 missions received from Drax.
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| Electro | Complete the "A Shock Withdrawal" bonus level.
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| Frost Giant | Complete level 7 "Bifrosty Reception".
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| Galactus (Playable) | Complete level 15 "The Good, the Bad and the Hungry".
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| Gambit | Complete three of Gambit's missions".
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| Gamora | Complete Story mode, then complete the first missions received from Drax.
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| Green Goblin | Complete level 9 "Doctor in the House".
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| Groot | Complete Story mode, then complete three missions received from Groot.
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| H.E.R.B.I.E. | Complete level 2 "Times Square Off".
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| Hawkeye | Complete level 3 "Exploratory Laboratory".
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| Howard the Duck | Complete the "Nuff Said" bonus level.
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| Hulk | Complete level 1 "Sand Central Station".
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| Human Torch | Complete level 6 "Red Head Detention".
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| Iceman | Complete level 8 "Juggernauts and Crosses".
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| Invisible Woman | Complete level 9 "Doctor in the House".
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| Iron Fist | Complete the race mission with Blade, then win the fight with the ice enemies in the Blade mission.
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| Iron Man (Heroic Age) | Complete the "New York Event Deadpool" bonus mission.
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| Iron Man (Hulkbuster) | Land on "S" sign landing platform, then destroy all airvents around the "S" sign.
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| Iron Man MK I | Complete level 5 "Rebooted, Resuited".
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| Iron Man MK VI | Complete level 1 "Sand Central Station".
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| Iron Man MK VII | Complete the "House Party Protocol" bonus level.
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| Iron Man MK XLVII | Complete level 5 "Rebooted, Resuited".
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| Iron Man MK XVII | Complete the "House Party Protocol" bonus level.
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| Jean Grey | Complete level 8 "Juggernauts and Crosses".
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| Juggernaut | Complete level 8 "Juggernauts and Crosses".
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| Kraven the Hunter | Collect the Kraven token by shooting the five targets next to Godzilla-type icon at Central Park.
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| Loki | Complete level 15 "The Good, the Bad and the Hungry".
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| M.O.D.O.K. | Complete level 10 "That Sinking Feeling".
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| Magneto | Complete level 13 "Magnetic Personality".
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| Maria Hill | Complete Maria Hill's three missions on the Helicarrier.
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| Mister Fantastic | Complete level 2 "Times Square Off".
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| Mysterio | Complete the "Thrill of the Chess" bonus level.
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| Mystique | Complete level 12 "Rapturous Rise".
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| Nick Fury | Complete level 9 "Doctor in the House".
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| Nova | Complete the foot race mission with him to the east of the Godzilla-type icon at Central Park.
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| Professor Xavier | Complete Professor Xavier's three missions behind the X-Mansion.
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| Psylocke | Complete all Captain Britain's missions.
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| Pyro | Complete level 8 "Juggernauts and Crosses".
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| Red Skull | Complete level 6 "Red Head Detention".
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| Rhino | Complete level 12 "Rapturous Rise".
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| Rocket Raccoon | Complete three missions: Garbage truck northwest of Central Park, just east of the Feeling Fisky Bonus Mission, 3 or 4 blocks south of the east coast.
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| Ronan the Accuser | Collect the Ronan character token by finding hidden path behind the statue south of his icon.
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| Sandman | Complete level 1 "Sand Central Station".
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| Silver Surfer | Complete three Silver Surfer missions.
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| Spider-Man | Complete level 1 "Sand Central Station".
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| Spider-Woman | Collect the Spider-Woman token west of the park on the southern-most part of the island.
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| Squirrel Girl | Collect the Squirrel Girl token on the docks northwest of the "Put Up Your Dukes" bonus mission.
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| Stan Lee | Rescue all 50 Stan Lees.
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| Star-Lord | Complete three missions from Star-Lord.
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| Storm | Complete level 8 "Juggernauts and Crosses".
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| Symbiote Scientist | Complete level 3 "Exploratory Laboratory".
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| The Destroyer (Playable) | Complete level 7 "Bifrosty Reception".
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| The Mandarin | Complete level 5 "Rebooted, Resuited".
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| Thing | Complete level 9 "Doctor in the House".
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| Thor | Complete level 7 "Bifrosty Reception".
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| Tony Stark | Complete level 5 "Rebooted, Resuited".
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| Tony Stark (Underwear) | Complete level 4 "Rock up at the Lock up".
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| Union Jack | Complete "The Brick Apple" bonus level.
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| Venom | Complete level 3 "Exploratory Laboratory".
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| Wasp | Collect the Wasp token one block south of the Oscorp Building".
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| Wolverine | Complete level 4 "Rock Up At The Lock up".
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