Haven't seen him in much else, but Jamie Dornan was really good in Season 1 of The Fall ...
I've always loved Patrick McGoohan, especially in The Prisoner ... he had the cool factor, obvious intelligence and acting chops. But he might have been a little too intense at times for Bond, who should (at least for me) have a debonair, laid back, slightly louche quality.
Cary Grant (the Best Man at future Bond co-producer Broccoli's wedding) might have done the first Bond, except the producers wanted someone contracted for five films--a later sore point for Connery.
Similarly, Hitchcock might have directed the first film, if we can believe the stories; but the producers (Saltzman was from Quebec, btw) probably thought he (and Grant) were too expensive.
Of course, if Hitchcock had done it, it would have been a "Hitchcock picture," not exactly what they had in mind, even if Hitchcock's North By Northwest, with Grant, is the obvious template for cinematic Bond, which would later steal a variation on the famous crop-dusting scene for FRWL.
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