It would help if you gave some idea what you already have and have played. A decent, similar thread for PS2 recommendations is RAB's recent one:
http://www.gamingforce.com/forums/so...r-console.html
I second chao's recommendations for ICO and Katamari.
Both
Katamari Damacy games are essential PS2 purchases. Quirky, extremely funny and brilliant in design and execution, not to mention awesome soundtracks. They have the kind of respect and love for games and gamers alike that are so missing from most console titles these days, and they remind you why you play games in the first place.
ICO is the very definition of gem. Relatively small in scale, but beautiful in execution (and I don't only mean the graphics). A wonderfully elegant title and different take on the platform adventure. Also my personal favorite console game ever and in my opinion the Playstation 2's finest.
From GBA, I'm currently going through
Legend of Zelda - Minish Cap and it's absolutely brilliant. I was worried it would feel tired and calculated, especially after replaying the magnificent Link to the Past, but Capcom's take is wonderful, familiar enough to feel safe, yet new and clever enough to feel fresh and costantly surprising you pleasantly. It's a terrifyingly addicting game though, so be warned.
Before Minish Cap, I finished
Mario & Luigi - Superstar Saga, which was awesome. One of the funniest games I've ever played, a wonderfully witty and clever action-RPG, that loves games and Nintendo, but is not afraid to poke fun at either. If you've played your fair share of Nintendo classics, there's a massive amount of humor to be discovered in the story and settings, constantly embracing and making fun of Mario cliches and video game conventions alike.
For PC, I seriously recommend playing
Grim Fandango, if you haven't yet. A brilliant, extremely stylish and witty adventure game, with a superb script, cast and soundtrack. Some of the greatest dialogue in games ever, and my favorite PC game. Some of the puzzles can be a bit obscure, but they all consistently follow the gameworld's logic.
Jam it back in, in the dark.