No, but this was a very good try: I found a picture of this guy too, whilst searching through Danger Man, The Saint and The Prisoner earlier. I'm pretty sure now the crazy baldhead I'm looking for turned up in the latter as well (I can see him in a dark blazer with a white crew-neck jersey).
They seemed to alternate between the bald guy and Bert Kwouk for villainy,
but he's another bowl of noodles...