Funny I was thinking about this too the other day...
Connery had the better movies IMHO, as Moore's degenerated into flash filled spectacles (see Moonraker
). And Moore was too smooth. He didn't come off as a killer, most of the time. Add to that by the time the last Moore movie came out, he was nearly 60, and moved like it. Connery had that gleam of barely suppressed sadism and aggression that lurked right beneath the surface (see the fight in Goldfinger
against the SPECTRE agent that killed 008). Which seemed to fit the Bond character so much better. I mean he is supposed to be a secret agent/assasin, not a millionaire playboy. I never really had time to forge an opinion on Dalton, 2 movies just weren't enough. Lazenby was decent, not great and had potential, but never followed through.
Greatest Connery film(in the series): From Russia with Love
Greatest Moor film: The Spy Who Loved Me
but you've really got to see the whole canon to truly see Bond...
*the above is merely opinion, take it as you will*