N64 was the first home console I bought due to being pretty much a PC-only gamer prior to that. Bafflingly the game that made me want to buy it was Pokemon Stadium
What a pile of gooseberry fool that was. Still, so many other games made it so worthwhile - the likes of Mario 64, Ocarina of Time etc. blew me away and as much as anything offered something wildly different to what I could get on PC. Most of my school friends owned N64's too so I got to experience a lot of games by borrowing through them.
It remains one of my favourite systems of all time and still gets pulled out from time to time to play Goldeneye/Mario Kart 64, which despite both being horrendously slow now are still great fun in 4-player in my opinion.
Playstation was great but I never owned one, although I played FF7/8/MGS on my PC and they're all amongst my favourite games, not to mention I later went out and picked up some of the back-catalogue when I owned a PS2/3. Was a wonderful machine and there's a lot of games I missed out on due to not owning one.
Think I'm going to have to go for the N64 purely because I owned one and its exclusives were superb whereas many of the PS1's best games I managed to play superior versions of on my PC.