If you're talking about all time, Goldeneye for N64 would probably be my favorite, but it's a tough call. If you're talking about current, Bioshock or Mass Effect for single player. Halo 3 for multiplayer.
As many others have said, it really comes down to how much you like multiplayer. I beat Bioshock twice, and in terms of a single player game, it's probably the best game on the 360 to date. I've already spent more time playing Halo 3 because of the multiplayer, but if I had to choose one it would probably be Bioshock, simply because it is a more unique experience, and because I can only play a multiplayer game for so long before I get tired of it. I may change my opinion after some time however, seeing as this already is the most I've played a multiplayer game this much since Goldeneye for N64.
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