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N64 by a mile. Admittedly, this is from someone who only played both sporadically on my friends consoles but N64 games were simply a revolution for the time. Goldeneye alone was the first FPS to work on consoles and even the N64 versions of PC FPS' seemed to work really well on the console (e.g. Quake II). Then you had Mario 64, OoT, Lylat Wars, Perfect Dark etc. to keep you going.

Basically, Nintendo managed to pull off the near impossible task of getting their 2D franchises to work perfectly in a new 3D environment whilst releasing some top new exclusives that were the envy of every Playstation/Saturn gamer. Like I said before, N64 games were a revolution. That simply didn't happen on Gamecube.