I think Goldfinger or From Russia With Love will come out on top. Both of those films are the best, if not THE best, in the series.
Dalton, Moore, Brosnan, Lazenby, and Craig all have their films, but nothing comes close to Goldfinger or From Russia With Love. Dr. No is also a great film, but it's somewhat of a paragon at this point in the series.
I'm not a fan of Moore at all. Though, He does have some decent offerings; Live and Let die; The Spy Who Loved Me; Octopussy.
Lazenby has the look but can't act very well. On Her Majesty's Secret Service is a film that has aged well with time.
Dalton is, probably, my all-time favorite Bond. The Living Daylights and Licence To Kill aren't very good movies; but Dalton's performance makes up for it, serious, cold and cruel -- a true Fleming's Bond.
Now, Brosnan. . . there's a guy who had some potential. Too bad he got lousy movies after Goldeneye. I think he combined everything the previous actors did on screen -- Connery, Lazenby, Moore, Dalton -- and put it all into Goldeneye. Some people don't like Goldeneye (and don't like Brosnan all too much for that matter), but I think it's a darn good film in the series.
And now the battle begins. . .