Easily Merc 2...
Army of Two is a very linear game... Pretty good but not great... More "forced co-op" scenarios but some new ideas to the FPS co-op concept... I didn't find the story that great though and felt the game was never really completed to what it could be.
Merc 2 is a fun open world game. It will last a lot longer and it is a lot of fun to just take out an RPG and blow something up because you want to... There are many different mission types (Take over an area, capture a high value target person, destroy a well protected building, etc.) and some challenges (Shooting targets with different weapons, races, grappling with a helicopter, experimental vehicles tests, etc.). Lots more types of weapons and more variety in how you can do missions at your own pace and how you want to (Call in air strikes, air support, etc.).