It has been regarded by some music critics as the finest-sounding LP of all time. The original album cover art was done by Robert McGinnis, based on the film poster and the original stereo vinyl release of the soundtrack ( Colgems #COSO-5005) is still highly sought after by audiophiles. At the time, Barry was the main composer for the Eon Bond series.

John Barry's song ' Born Free' was also used in the film. To make room for her credit in the film titles, the credit for Jean-Paul Belmondo was removed in the German language version. The German version of the film, however, features a German adaptation of 'The Look of Love' sung by Mireille Mathieu. Springfield's version was heard again in the first Austin Powers film, which was to a degree inspired by Casino Royale. A year later a version by Sérgio Mendes and Brasil '66 reached #4 of Billboard Hot 100. The song was a Top 10 radio hit at the KGB and KHJ radio stations. 'The Look of Love' was nominated for the Academy Award for Best Song. It is played in the scene of Vesper Lynd recruiting Evelyn Tremble, seen through a man-size aquarium in a seductive walk. The 4th chapter of the film features the song ' The Look of Love' performed by Dusty Springfield. (A version of the song was also sung by Peter Sellers.) The title theme was Alpert's second number one on the Easy Listening chart where it spent two weeks at the top in June 1967 and peaked at number twenty-seven on the Billboard Hot 100. Herb Alpert & the Tijuana Brass performed some of the songs with Mike Redway singing the lyrics to the title song as the end credits rolled.

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