1. Sean Connery
2. Roger Moore
3. George Lazenby
4. Timothy Dalton
5. Pierce Brosnan
^ I've seen all 007 movies with these gentlemen, incl. the funny Thunderball remake Never Say Never Again.
Connery was the best and most charismatic movie actor by far, which he proved throughout his career with roles in great movies such as The First Great Train Robbery, The Man Who Would Be King, Robin and Marian, Outland, The Untouchables, The Name of the Rose, Indiana Jones and the Last Crusade.
But imo Connery also benefitted from the facts that
- he was the first 007
- the best Bond movies were created in the cool 60s when he played the character (Goldfinger, From Russia With Love, Thunderball, You Only Live Twice), which made 007 and himself pop culture icons.
Lazenby was a bit overextended even with this role, but like all Bond movies from the 60s On Her Majesty's Secret Service was great fun (and he had Diana Rigg!).
Moore was the last Bond I really liked, it took some time though...but in the end I learned to appreciate his understatement and self-mockery.
I haven't seen a Bond movie with Daniel Craig yet, but I'm not really interested in Bond movies anymore. The mass media said the same thing about Craig this decade what they said about Dalton in the 80s and Brosnan in the 90s: "Bond reinvented !"