3. 'You Only Live Twice' (Nancy Sinatra)
The rising whirl of strings that kicks off this formative 1967 Bond theme might just be John Barry's finest moment (even if it was lifted from an Alexander Tcherepnin concerto, the decision to use and tweak it here is still a stroke of genius). Originally intended for Frank Sinatra but ultimately delegated to his daughter, "You Only Live Twice" is located somewhere in the Bermuda Triangle between James Bond and South Pacific. Playing off of the film's Japanese setting — yes, this is the one where 007 fakes his death and comes back to life in yellow face — Barry augments a breezily majestic melody with the exotic plink of bamboo xylophones, and Nancy Sinatra's voice trembles around them in style. More recently, the season five finale of Mad Men confirmed what audiences of the time knew right away: This song is a classic.