Enslaved Odyssey to the West, Bioshock 1&2, Prototype, Alice Madness Returns, Left 4 Dead 2, Fatal Frame 2 (I THINK you can get it for the Xbox), any of the Silent Hill games, Alan Wake, Hydrophobia, Mirror's Edge, ... d'awww, drawing a blank now...
If you're into action games, Bayonetta is pretty good (the superior version is on the 360). Fast paced, over the top, and endlessly satisfying. Also good if you're looking for a fair challenge.
If you're looking for a unique experience try Dark Souls. Its brutally hard but its one of the best games I've ever played. Also, I second the recommendation for Banjo Kazooie: Nuts and Bolts, awesome game.
Shadow Complex is good. Lost Odyssey is awesome if you like JRPG
The Mass effect series is amazing. Elder Scrolls games are brilliant. Dead Rising 2 is worth checking out.
I also really like the Fallout games on 360
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