Most PS1 and N64 games haven't aged too well mostly due to the fact that a lot of them were running at around 15-20 frames per second. We may not have noticed that in the past but it feels nigh on unplayable now due to how unresponsive and laggy everything feels. Goldeneye has already been pointed out but basically anything that would require fast reflexes and precise controls just don't play too well today. Thankfully there are emulators to allow one to bypass those frame rate problems :)
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http://gamercards.exophase.com/4831.png
http://i51.tinypic.com/2zpi5w4.png <-- How I look as per Clogged_Artery (Thanks!)