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Resident Evil (original)
Has a creepy, unsettling atmosphere, helped by a superb soundtrack and a general sense of discovery as the story slowly unravels.

Tomb Raider (1996)
Really captures the feeling of isolation and wonder. The silence occasionally punctuated by musical cues is really effective.

Twilight Princess
I feel like there's a sense of foreboding running through this game. I dunno, the world just feels kind of bleak and unsettling to me.