Dude go buy Persona 3 portable, even if you haven't got a PSP yet go buy it.
Then get Crisis Core, Dissidia, Final Fantasy 4, Kingdom Hearts, Parasite Eve, Gran Turismo, Tactics Ogre, Ratchet and Clank and Peace Walker. Oh and Patapon if you have money left.
Symphony of the Night (actually it might be better to just buy Rondo of Blood's remake Dracula X for the PSP. Since that comes with both the prequel Rondo of Blood remastered and Symphony of the Night bundled into one complete game)
Metal gear peace walker is the best one hands down.
Valkyria chronicles 2 very good, a lot of content, solid turn based RTS.
Dissidia 012 Final Fantasy very good fighter.
Patapon is a very weird yet addictive rhythmic game with rts strategies.
Crisis Core: Final Fantasy VII good story and fun gameplay
Metal Gear Solid: Peace Walker is pretty much all I ever use my PSP for. You probably won't have the necessary back ground info if you haven't played MGS3 though...
I haven't many games for my PSP, but of them I can heartily recommend Loco Roco, a fun game where you control a little yellow blob which you must escort to the end of the level. It isn't terribly difficult, but I think the soundtrack is pretty good and it has a rather calm and relaxed atmosphere.
Well since you don't want JRPGs there goes my big recommendations(Persona 3 Portable, Kingdom Hearts Birth By Sleep, Disgaea 1 and 2, and (even though it's more fighting game than JRPG) Dissidia 012: Duodecim).
Hmm...gonna say go for Metal Gear Solid: Peace Walker, whatever the newest Monster Hunter game on it is, and Castlevania: Symphony of the Night.
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