Find their tokens around the city and purchase them at corresponding vehicle call-in points: Land for cars, water for boats, helipads for planes and helicopters.

Vehicle	How to unlock
Captain America's Bike	Taxi the character at the Dockyard to his destination.
Chitauri Chariot	Unfreeze 4 citizens who are frozen by Loki in Times Square.
Deadpool's Helicopter	Complete a Deadpool mission in West Harlem.
Deadpool's Scooter	Defeat Deadpool in a race on the Brooklyn Bridge.
Doom Jet	Collect its token in the Financial District.
Fantasticar	Collect its token atop a fountain in Central Park.
Flower Car	Complete a Groot quest in Central Park.
Garbage Truck	Complete a Roccet Raccoon quest in the Scrapyard.
Ghost Rider's Motorcycle	Defeat Ghost Rider in 3 races..
Go-kart	Defeat Maria in a race on the SHIELD carrier.
Golf Cart	Collect its token on Liberty Island.
Hydra Tank	Collect its token atop the Empire State Building.
Magneto-mobile	Complete a Professor X mission at the X Mansion.
Mandarin's Boat	Complete a Groot quest in the Financial District.
Mandarin's Buggy	Collect its token in the Industrial District.
Mandarin's Helicopter	Complete a Gambit mission at the X-Mansion.
News Helicopter	Collect its token above the tunnel in the Upper East Side.
Pizza Bike	Defeat Blade in a race beginning in the Financial District.
Pizza Van	Collect its token in a store in Little Italy.
Police Helicopter	Shoot four targets in the Industrial District.
Police Motorcycle	Collect its token in Yorkville.
Police Truck	Collect its token at Horizon Labs.
Pumpkin Chopper	Collect its token atop the Oscorp Building.
Punisher's Car	Complete Punisher's mission after unlocking his truck.
Punisher's Truck	Complete Punisher's first mission.
Raft Helicopter	Collect its token on The Raft.
Raft Truck	Collect its token at The Raft's island.
Raid Truck	Beat Whack-a-mole game at The Raft Ferryport.
S.H.I.E.L.D. 4x4	Collect its token in the Upper West Side.
S.H.I.E.L.D. APC	Collect its token in a building at the Raft.
S.H.I.E.L.D. Jetfighter	Collect its token on the deck of the SHIELD Helicarrier.
S.H.I.E.L.D. Minicarrier	Complete a Maria quest on the SHIELD Helicarrier.
S.H.I.E.L.D. Staff Car	Collect its token atop a building in the Financial District.
Spider-Copter	Destroy three spider webs atop Ant-Man's lab.
Spider-Cycle	Collect its token atop Sanctum Sanctorum.
Spider-Trike	Collect its token in a greenhouse in the Upper East Side.
Stark Jet	Collect its token in the water in Central Park.
The Britmobile	Complete a Captain Britain quest in the Financial District.
Wolverine's Motorcycle	Complete a Toat quest in Industrial District.
X-Jet	Collect its token in a cave under the X-Mansion.