Try Final Fantasy Tactics: the War Of the Lion, it is kinda an auto response from me. But it may not be a game for everyone, it is a polished re-release of the classic from 1997. It is the reason why I own a PSP myself.
Should also try out re-release of original FF and FF2 which are very nice games. Retro - but still nice to play if you haven't. It is like playing old game history, to see where Square started with their Final Fantasy franchise.
Look how basic and simple it was back in 1987. They pushed the hardware abilities already then.
These new releases are of course fixed up for the PSP and edited a bit with new sound.
This is only if you like RPG games of course.
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PS3: DMC4, Uncharted, Heavenly Sword, Ratchet & Clank, Assassin Creed, Folklore...
PSP: Final Fantasy 1, 2 and Tactics.
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