PS1 by far. Resident Evil 1-3, Dino Crisis 1 and 2, Final Fantasy VII-IX, Metal Gear Solid, Parasite Eve 1 and 2, Twisted Metal 1-4, Silent Hill, Syphon Filter, Tekken 1-3, Tomb Raider 1-5, Chrono Trigger and Cross, Spyro the Dragon, Legacy of Kain, the list goes on and on.
PS1 was leaps and bounds better.