I’d give top 10 to N64, but admittedly haven’t played many on either system.
N64: Mario Kart 64, Goldeneye, all the Mario Party’s, THPS 1&2 (played them on N64), Mario 64, Mario Golf, Mario Tennis, Perfect Dark.
PS1: Metal Gear Solid, Lunar Silver Star, Twisted Metal 1&2, NFL Blitz, Medal of Honor & Underground, Unholy Wars, Worms Armageddon.