Shadow of the Colossus, Fumito Ueda's magnum opus, is one of the greatest games ever developed. However...the PS3 remaster, which also includes a remaster of Ico, is superior to the original (which has frame rate problems, among other things), so I'd wait for a PS3 for that. The same goes for Metal Gear Solid 2 and 3, and God of War 1 and 2 -- I haven't played their remasters, but the same developer, Bluepoint Games, handled all of them.
Some other good ones for the PS2:
Okami
Katamari Damacy (quirky beyond belief but also addictive beyond belief)
Devil May Cry (I haven't played any of the sequels, but I did like this)
Silent Hill 2 (I didn't play the first one, but I did like this)
Final Fantasy X and XII (there's been some backlash against XII, but it's not a terrible Final Fantasy)
Valkyrie Profile 2 (only if you've played the first)
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