This topic is slightly old, but I still wanted to offer some imput.
The Gamecube might just rank as my favorite console (although the PS3 is coming close to overtaking it). Just some highlights:
Various Zelda titles. They're always a prime Nintendo series and there are a number of options for the Gamecube
Resident Evil 4. It started off as a Gamecube exclusive, before an expanded PS2 release. I still pick the Gamecube version as THE version to play as the controls simply feel better. Graphics are a bit better, also.
Speaking of Resident Evil, there is Resident Evil Zero, plus Resident Evil REmake, and RE2 and RE3, not to mention Code Veronica. And maybe one or two others I'm forgetting.
Mario Kart Double Dash, in addition to a whole menagerie of other Mario titles.
Metroid Prime is the FPS that everyone WISHES they could play. But they can't without Gamecube. Pity.
Ikaruga is considered a must-play, although I personally have not found the reviews to mention anything that I am interested in.
Eternal Darkness: Sanity's Requiem might be the best exclusive on the Gamecube. Widely considered to be one of the more creative and interesting horror game around. I consider it to be a must-play and well-worth the price of the system alone.
I have played multiple versions of Lego Star Wars, and the Gamecube is by far the best of the lot (with a close 2nd to the DS version). Wholly satisfying and a ton of replay value.
Chibi-Robo! is one of those games that I have not personally played, but it looks awesome. There are a bunch of random games like this for the game cube that only Nintendo would OK.
F Zero-GX is one of the best and hardest of the space racers. Looks gorgeous and highly recommended.
Killer7 is an odd game that rides the line between FPS and horror with a distinct comic-book style. Another highly underrated game.
Beyond Good and Evil is multi-plat, but a very solid part of the Gamecube library.
So many others, I haven't even gone through half of the list. But I got bored. Soooooo...
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