My top three would be Goldfinger, On Her Majesty's Secret Service and GoldenEye.
Really, OHMSS gets a bad rap because of (the underrated) George Lazenby; it's the most cynical of the franchise, one of the most brutal, and has stunning cinematography and set-pieces. If they ever start to remake them, this should be the one.
I also quite like GOLDENEYE as well. Before ROYALE, EYE was the last 007 flick that was good on its own deeds outside of the 007 brandname. No coincidence that both were shot by Martin Campbell. No Sir Yee....
As for OHMSS, I always liked it. Not the biggest fan of fucking Kojak as the villain, but otherwise its a pretty good and, as you said, brutal(for a 007 flick) that really promised the next 007 installment to be where a pissed-off vengeful Bond was out to exterminate Blofeld and S.P.E.C.T.R.E. once and for all.
Too bad Eon Films fucked that all up on DIAMONDS ARE FOREVER.
