Daggerfall dungeons; game set on very high reflexes.
^You are a very brave man.
I would say Dead Money, but other than the Holo-guards it never really got to me. Too much Silent Hill, I suppose. Its still my favorite DLC of all time, because the characters were amazing.
Vault 22 was pretty unnerving once you notice that
Spoiler some of the infected you've been killing are children.
Vault 11, at the very end, had me so enthralled that I only just realized some [censored] was about to go down a few seconds before it hit the fan.