My vote for the best villian laugh: The Hooded Claw from the Perils of Penelope Pitstop definitely had a great laugh, plus he was a master of disguises, for a villain that's a pretty handy skill. Related to that topic, I always thought it interesting that Paul Lynde's name was never listed in the end credits, I have a theory about that. Back in the late 60's and most of the 70's as most everyone knows Paul was the center square on NBC's The Hollywood Squares during the daytime on weekdays, plus in '69 he was the voice of the Hooded Claw on CBS' Penelope Pitstop on Saturdays. I think the reason he never was listed in the credits is because CBS didn't want it known that someone from a rival network show on weekdays was doing a voice on a cartoon show for CBS on weekends, of course that's just my opinion. By the way, honorable mention for best villain laugh: most of the villains from Scooby Doo over the years especially the Phantom from the Scooby Doo Where Are You? episode "Hassle in the Castle", now he had a great laugh.