I'd say Timesplitters 2 and Timesplitters Future Perfect are the most fun co-op/multiplayer games for ps2. Baldurs Gate Dark Alliance is also fun. One that hasn't been mentioned is Lord of The Rings: Return of The King. It's another hack and slash type game.
Pretty much any of the rhythm games would be fun co-op if you're in to those types of games. Guitar Hero, SingStar, and Rock Band would all be good choices, albeit expensive choices. Racing games are fun co-op as well, so titles like Burnout and Gran Turismo could also be enjoyable. There's always sports games; Basketball, baseball, football, boxing, soccer, hockey, golf. They're all fun multiplayer games too. I guess it just depends on your taste and your budget. Happy game hunting. :)
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