Don't know about "scary", but the best horror game I've ever played is Shadow of the Comet. It's like it was made by Lovecraft himself - spooky, intellegent, with lots of story twists and horror thingies. Along with Alone in the Dark of 1992 it is among my top games.
As for scary, I'd go for Dark Corners of the Earth, Scratches and Amnesia. All of them have plenty of great moments and deserve their place in the industry.
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