They were both great, but N64 had Donkey Kong 64, Super Mario 64, Super Smash Bros., Paper Mario, Mario Party 1-3, Ocarina of Time, Majora's Mask, Mario Kart 64, Mario Tennis, Mario Golf, and a few more legendary games so yeah, that.
I LOVED both consoles, but N64 wins it. So many perfect games to this day. Me and my roomates even bought a used N64 and games just to play it again recently.
Some great games for both in my life were...
N64:
Super Smash Bros
Mario Kart
Legend of Zelda Ocarina of Time
Super Mario 64
Donkey Kong 64
Paper Mario
Pokemon Stadium 1 and 2
Pokemon Snap
Stars Wars Episode 1 Racer
Yoshi Story
Mario Party 1-3 (Especially 3)
(So much iconicness and a lot of my fave games)
Playstation:
Crash Team Racing
All Crash Bandicoot games
Spyro Games (Particualrly Riptos Rage)
Digimon World
Twisted Metal Games
Dino Crisis Games