I'd say Goldfinger. The villains (Goldfinger and the crazy Oddjob being both funny and sinister) are awesome, the plot has some nice twists, we see Aston Martin action (yay!), there are many memorable scenes, John Barry's score rocks, the theme song by Shirley Bassey is catchy, Bond gets to say some of the funniest one-liners, the dialogue itself is quite sharp, and of course there's this great mystery and action which makes Goldfinger a very good Bond film.