My wife and I are doing the exact same thing! I LOVE this thread!
Dr. No - the biggest letdown for me is relatively minor, and it's how Dr. No dies with such little fanfare - almost treated like any other henchman death.
From Russia With Love - I really like seeing how the Bond elements I took for granted (I was born in '73 so I too saw Moore as Bond first, bummer!) start establishing themselves. Seeing Q, the gadgets start to appear... the quips start getting funnier, and my god, the sexual double-meanings to some of the dialogue - so brilliant!
Goldfinger - Probably the best Bond villain, as he seems to get MORE dangerous as the film progresses, and it heightens the stakes.
Thunderball - Agreed that the underwater scenes start to get a little excessive, but only a little. I really do like to relax in a composed scene.
We just watched You Only Live Twice this evening... so I'll respect the wishes to keep current with ya!
Transfers are STUNNING. These look almost like contemporary films set in the 1960s, not made in the 1960s.
Favorite quip so far: "See you later, irrigator"