As for my faves (both my fave films by each actor and the actors are in the order that I best like them)...
Moore - For Your Eyes Only
Dalton - License to Kill
Connery - Goldfinger
Brosnan - The World is Not Enough (sorry, but GoldenEye bored me to tears)
Lazenby - haven't seen it, but I'm guessing my pick would likely be OHMSS (duh)