Doom 64 no question. Graphics were unnecessarily dark, but it was atmospheric and spooky, even more so than the PC versions.
Goldeneye was ok, but didn't really impress me, especially since I had already played much better FPS's on my PC, like Doom, Doom 2, Quake, and Duke Nukem 3D.
I rented Perfect Dark once and it was just meh, didn't motivate me to buy it.