In the Best Original Song category, I'm proud to Select, from 1961's Breakfast at Tiffany's, Moon River -- Music by Henry Mancini, Lyrics by Johnny Mercer. Damn, this is a gorgeous song; this would be a favorite movie of mine were it not for Mickey Rooney's offensive asian landlord which sours the entire film somewhat, but when it comes to songs, few work as well both on their own and in the context of the movie as well as Moon River.
It's great on it's own with Holly sitting on the balcony, but I love how Mancini uses the theme from it during the final scene of the movie:
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