I think so - the only serious competitors for the title that I can think of are the soundtracks for Tarantino's Pulp Fiction and Scorsese's Mean Streets.
Stanley Kubrick was widely acknowledged as a master of selecting just the right music for his films, a gift that is nowhere better demonstrated than it is here.
Can you really picture anything other than "Also Sprach Zarathustra" accompanying 2001's title sequence? Anything other than "The Blue Danube" running behind the film's first spaceflight scene?
The reals gems here, however, are the stunning pieces by Gyorgy Ligeti. His "Requiem..." is probably the most disturbing piece of music I've ever heard; his "Adventures" (best heard in its unaltered version, which is thankfully included) among the most suspensefully comic.
Highly recommended to anyone with a passion for great music.