From Russia With Love's score is pretty damned good, especially when you compare it to what we received in Doctor No. James Bond with Bongos has so much retro swag it's not funny. IMO, they couldn't replicate this atmosphere if they tried. Other tracks I really dig are Death of Grant and the Opening Titles. FRWL also introduced the 007 Theme, and I think that counts for a lot. I prefer Barry's other scores, but for a first effort, it's amazing and it immediately set the standard. It only got better from there.
The James Bond Radio podcast recently reviewed the FRWL soundtrack. Highly recommended listening.