Bond is a literary character. Craig and Dalton are best at portraying the literary character.
Connery did a great job with it but incorporated a lot of humor into his work. That defined who and what James Bond was to general audiences. And there's nothing wrong with that! The first three he was in are great! The last three? Garbage I clump with Roger Moore's films. Roger Moore might have been a great Bond if his films weren't so ridiculous. I've seen a handful and can't stand them. Pierce does the best job emulating Connery and is in one of the greatest Bond movies ever. His first two sequels are pretty fun too, not perfect, but not insulting. Than DAD came along...
Anyways, here's a list of ones I enjoy enough to watch multiple times:
Dr. No
From Russia With Love
Goldfinger
Goldeneye
Casino Royale
Quantum of Solace
I have not seen ALL of Moore's movies, OHMSS, or The Living Daylights yet.