So I've watched Dr. No through Goldfinger at this point. They all possess a pretty consistent quality, so I don't think any which one stands greatly above or below the others.
I think I liked Goldfinger the most, just for all of its Bond-isms that I know through years of. I also liked that the villain had an established presence throughout the film and encountered Bond several times. Really makes for a good nemesis. That said, even though I went into these films bracing myself for very dated portrayals of social norms, I've got to give a special hoo boy to the fact that Goldfinger's plot failing hinged on Bond forcing himself on Pussy Galore. There was some bad stuff in the first two, but I think this takes the cake.
I'll give second best to Dr. No, because I kind of liked its slower, more methodical pace, and the mystery of its villain. The setting was nice too, though again things are shaky with the portrayal of other cultures. Some of it wasn't as bad as I was expecting, but the yellowface was pretty egregious.
From Russia With Love was fine too, though I didn't enjoy the villain side of things. It was at once too explicit for the audience and not explicit enough for the characters. I'm not sure why, but the tension I should have gotten knowing that Bond was being stalked unawares just wasn't there for me. I did like his banter with Kerim Bey, but the stuff with the gypsies felt as if it's only purpose was to show us some belly dancing and have a catfight. None of this is to say I didn't enjoy the film though, just explaining why I didn't like it quite as much as the first two.
Dated values aside, they were all entertaining, and I look forward to more. I'm going to try not to skip any, just so I can view the full legacy for myself.