Depends how we're defining 'sound track'. From wiki:
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A soundtrack, also written sound track,[1] can be recorded music accompanying and synchronized to the images of a motion picture, book, television program, or video game; a commercially released soundtrack album of music as featured in the soundtrack of a film, video, or television presentation; or the physical area of a film that contains the synchronized recorded sound.
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For the first definition, I'd go with Alien (1979). The music and sound effects are both effective and blended so well, and with the images of the film.
For 'horror film' song, definitely "Sacred Springs" from Mothra vs Godzilla (1964).
As for an album soundtrack for a horror film... I can't say I've purchased or listened to a lot of entire horror soundtrack albums. I like the cuts on the Halloween (1979) soundtrack.