I'd love to see something similar to Fallout 3's Dunwich Building.
For something to be scary first requirement is that it has to be dangerous, was more scared sneaking around as a thief in the palaces in Oblivion than in the Dunwich building in Fallout 3, played it at level 20 before I got Broken Steel so the ghouls was easy to kill, I sneaked so I usually saw them before they saw me.
In the castles I risked being arrested and had to make be very careful to avoid the guards and other npc as if I got caught trying to fight my way out would just give me a huge bounty.
Dangerous enemies are more important than a scary atmosphere even if it’s also important.
Then you searched for scraps in the steelyard in the pit was pretty scary as you had few weapons.
Best idea would probably be to capture the player so you had to escape without your equipment, yes it would be far easier for mages.