YOLT has by far the best Bond soundtrack. It's one of the the only two full Bond OSTs worth owning on LP/CD (Casino Royale 1967 being the other one). Contains the best piece of music ever composed for any Bond movie:
It's not only the best Bond soundtrack, but also in my top 3 John Barry OSTs (1. You Only Live Twice, 2. The Black Hole, 3. Midnight Cowboy).
The movie is nice as well, but not even in the top 3 of 60s Bonds.