N64 by a mile.
I loved the GC but the N64 easily had the genre creating software and at least in my part of US due to its multiplayer games like Goldeneye, Mario Kart, Smash Bros, various sports and wrestling games was a must have. Not to mention it was one of the last times Nintendo actually spread its wings and experimented with genres and IPs on a massive scale. Heck, the Xbox owes a great deal to the N64 since it pretty much inherited a good deal of N64 fans thanks to Halo, the sports games and some of those that went followed Rare.
Honestly, the only thing probably held the N64 back from dominating was the format, unlike with the GC where its actual appearance was a detractor and the Wii/Wii U where it was technically weaker then the competition. The GC while Nintendo's least successful console was great but it isn't touching the greatness that the N64. Heck most of the GC's most successful Nintendo games originated or were sequels to N64 classics.
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