Actors:
1) Connery
2) Dalton
3) Brosnan
Films:
1) You only live twice
2) Goldfinger
3) The Living Daylights
4) Goldeneye
I think the thing that ties all the Bond movies together and keeps that level of awesomeness between them though lies not with the actors or the writers but with this chap:
http://en.wikipedia.org/wiki/John_Barry_%28composer%29