Mine are "Goldfinger" and "You Only Live Twice" in that order until I watch YOLT and hear Nancy Sinatra sing the title song and I am taken back in time to seeing that film with my family in the 60s. It depends upon which one I last watched but those two are my favorites!
Dame Shirley Bassey owns the title song to "Goldfinger" and Honor Blackman as "Kitteh Galore" is just gorgeous but so too is Akiko Wakabayashi as "Aki". Both films are great and Goldfinger was the first Bond film for me.
I am now listening all of the Bond theme songs now. The music satisfies what passes for my soul.
This reminds me that I have the latest iteration of The Best of Bond... James Bond Limited Edition album in LP format (gold colored vinyl) on the way. Can't wait!