Just finished From Russia With Love. This has been my favorite for a while and I don't see any Bond movie topping it.
It has a brilliant opening, and a lot of great set-up and anticipation. The supporting characters are all interesting, and the film manages to juggle a lot of schemes and sub-plots without overwhelming the viewer. I noticed some nice camerawork and framing too...I dare say artsy.
The action in FRWL is quite good, although the fight scene in the train blows everything else away. It's one of the great fights in cinema, if you ask me.
If the movie has one flaw, it's that it lingers too long after that fight. @drbunnig identified this also. The whole movie is building toward the confrontation with Grant, and then we get 20 minutes more of escapes and fights. It's overkill.