Connery: TB (The swagger and charisma is at an all time high here. Best example: the scene where he humiliates Largo's henchman in the bathroom, then gives him his gun and throws the "little fish back. A great moment.);
Lazenby: OHMSS (While there's no choice here, he displays some pretty good acting at times for a guy who had never acted before.);
Moore: TSWLM (In his first two films, Moore was trapped between his natural instincts of how to play Bond and Connery's blueprint. For instance, cruelty always made Connery look menacing, but it just seemed mean when Moore played it that way. TSWLM is the film where Moore truly figured out how to play Bond his way. Although his later performances varied based on the tone of the film, TSWLM served as the template.);
Dalton: TLD (The lighter tone of this script prevented things from getting too serious, but there was still plenty for Dalton to sink his teeth into. Heavily influenced by Fleming, he gives one of the great performances of the series.);
Brosnan: TWINE (I agree with the consensus here. Brosnan was very convincing in this one. While I found his Bond to generally be rather dull, TWINE is the exception.);
Craig: QoS
(I realize this is controversial, but hear me out. Daniel Craig is given very little to work with here, yet he manages to squeeze water from a rock. His performance is very nuanced, but the film is paced so rapidly that it's only after repeated viewings that this comes through. He is a subtly able to convey anger, sadness, compassion, and grief. He's also very dynamic in the action scenes. He singlehandedly keeps the film afloat).