Hands down the best movie soundtrack in the history of movie soundstracks is Passion, Music from The Last Temptation of Christ by Peter Gabriel, don't buy anything else until you get this one.
Not necessarily a single best soundtrack, but I hope we wouldn't forget the film music of Bernard Herrmann. A good sampler to try would be Salonen's Los Angeles Philharmonic recording on Sony (SK 62700). A personal favorite would have to be "Taxi Driver", or any of the many Hitchcock movie scores which Hermann composed. Also check out the classic recording "Fantasy Film World of Bernard Hermann". Enjoy!
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