These are simply by my tastes. I actually watched Dr. No through YOLT today with some friends.
1) From Russia With Love - Overall, my favorite Bond film. One of the very few genuinely intelligent Bond films. Red Grant is great, I love the way he says "um-hmm" when answering Bond on the train. And a great fight between the two! Much better than the fight with Jaws in TSWLM.
2) Thunderball - So many people say this one lacks, and I can understand that view. The underwater sequence sometimes gets confusing as heck. However, I love this one. Great class, great villain, and all-around the best caliber of Bond girls in the entire series. Great poster and song as well.
3) Dr. No - Say what you will about it, it's one one of my favorites. It's a wonderful start.
4) Goldfinger - Am I the only who isn't that huge a fan of this movie? Sure, Goldfinger (the villain) is great, and so are Pussy and Oddjob. However, when it gets to Kentucky (my home state) it just lags to me, esspecially the battle at Fort Knox.
5) Diamonds Are Forever - What a bizarre movie! This is actually one of my favorite Bonds films (to watch). It's truely a unique (and fun) ride. I love this movie! I really do! It's stupid as heck, but I can't bring my to hate it!

It's odd really, if you did an evolution chart for Blofeld- (63-65): nothing but a hand a pu.. sorry, kitty cat (67) whiney little Donald Pleasance (69) Kojak (71) Charles Gray in drag. This film basically thumbed it's nose at the entire Bond franchise to that point. On top of that you have Wint and Kidd (whom I find very amusing) and Jimmy Dean the sausage king. Heck, Sammy Davis Jr. is one of the deleted scenes. Bizarre! Great score too.
6) You Only Live Twice - I'll just say it, I really don't like this movie. DAF was much, MUCH dumber, but at least it didn't take itself too seriously. YOLT gives me that impression. The plot just never goes anywhere to me. Plus, Bond never really goes anywhere, he always taken or lead somewhere. The Bond girls are also very unattractive. Nothing against Japanese girls, I've seen many attractive asian girls, but none of them are in this movie. Helga Brandt (IMO) seems "mannish" to me. I keep expecting Austin Powers to butt in and try to pull of her wig. YOLT is just boring to me. I have to say, however, that it has a beautiful score and title song.
I've only seen bits and pieces of NSNA, so I left it out.