I'm primarily a PlayStation Gamer, but I got one recently for some exclusives. Here are some noteworthy ones I was after:
Alan Wake
Blue Dragon
Bully: Scholarship Edition - Best Version
Burnout Revenge - Best Version
Cars - Best Version.. yes, really Cars

Condemned
El Shaddai: Ascension of the Metatron - A surreal game! I know it's one PS3 just throwing it out there.
Fable Remastered, 2 & 3 - great set of games!
Gears of War Series
Gun - Best Version
Halo 3, ODST, Reach & 4
Infinite Undiscovery
Kameo: Elements of Power
Last Remnant, The
Left 4 Dead 1 & 2
Lost Odyssey - One of the best JRPG's!
NieR - Recently boughtthis again, Love it!
Ninja Blade
Ridge Racer 6
Tales of Vesperia
Tenchu Z
Witcher 2, The: Assassins Of Kings - Enhanced Edition
Also, keep in mind that the console is backwards compatible with Xbox games like Fable, Crash Twinsanity & Shenmue II!