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I would say (The Fall of the) House of Usher (1960) and The Haunting (1963). Believe it or not, I watched those movies just a few months ago and they actually scared me. I didn't think movies from the 1960s could be scary, but,in my opinion, they actually were (don't get me wrong, there are plenty of great older movies, I just didn't think they could be scary).
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