I used ti love ThunderBall. Of course, not as much as a lot of other Bond films, but it was always in at least the top 5. After many recent viewings.. It's only gone down the list, and I expect it to only drop more. Little sad really, Connery does some fantastic acting, and has some good lines and quips, but the underwater action and other boring scenes... and.. some awkward ones.. Really drag it down from being so much better.
Goldfinger was the first Bond movie I saw, and I loved it. But.. it has really dropped, Bond doesn't really do much at all in the movie till the end, and so many other films just do things so much better. No doubt the iconic scenes are great and Connery does one of his few good acted performances.
GoldenEye was another one I really thought was the best one, and could never be topped. It still remains near the top, but I've really noticed it wasn't as good as I had believed.