Flexington,
If haven't played the God of War 1 and 2 from the PS2, they were digitally remastered and release don one disc for the PS3. You can get it for about $20 and they are absolute must plays for that system. The games hold up very well, considering how old they are. Then, of couse, God of War 3.
Also, Uncharted 2, Bioshock (FPS + puzzles) and Batman: Arkham Asylum and RDR.