This generation, my favorite co-op experience has been New Super Mario Brothers Wii. Though at times we were anything but cooperative. But that was a part of the fun.
Red Dead was another fun one.
Haven't played Portal 2, but I'm sure the co-op in that is a blast. Only drawback would be that after you play through once, there would be little reason to do it again, since you already know the solutions to the puzzles.
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