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N64 was a far superior machine. It's capabilities were far beyond the PS1. You only have to look at titles like Perfect Dark and Donkey Kong 64 to see far superior graphics. Also Zelda OOT is another example of massive jump in graphics over anyhting the PS1 had.

In terms of games PS1 had more games, but the N64 had the better blockbusters IMO.

The only game on PS1 that matched the quality of N64 was FF7.

PS1 had nothing that played as smooth or was as good as the following:

Goldeneye 007
Perfect Dark
Mario 64
Banjo Kazooie
Banjo Tooie
Mario Kart 64
Diddy Kong Racing
Zelda OOT
Zelda MM
Donkey Kong 64
F - Zero X
Killer Instinct Gold

The only genre where N64 lost out was JRPG's. But N64 blockbusters were amazing.