For the quality of the music alone, it would be West Side Story (1961) —Bernstein was on top form for that one. But for the best overall music + acting + story in a movie, I'd give it to Oliver! (1968).
If you've got an hour and a half to spare, here's an entertaining BBC documentary about a recording of the West Side Story music with Bernstein, Te Kanawa and Carreras.
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