Trivia Challenge: I see Richard Boone’s Hec Ramsay (another series in NBC’s “wheel”) is mentioned in that article. Boone is, of course, best remembered for playing Paladin in the TV version of Have Gun, Will Travel.
Who played Paladin in the radio version?
Well, it’s not a contest. There’s plenty of good bad guys in comedy.
But if I was to play Devil’s Advocate, I might say, amusing though it was to see a procession of semi has-been actors hamming it up as Batman villains, they weren’t necessarily all that funny as comedic characters.
Second-best Catwoman ever! 
All I know is, Julie Newmar as Catwoman caught my attention as a kid. I have little or no memory of the other two.
Julie Newmar
Eartha Kitt
Then Lee Meriwether
Let’s agree to disagree on this one.
So Michelle Pfeiffer would be fourth?
The Danby clan, especially Bruce Dern as Joe and Walter Brennan parodying himself as “Pa”, in Support Your Local Sheriff!
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Hedy Lamarr.
That’s Hedley!!
Of course you also have the 2nd tier/henchmen like Taggart and Lyle, plus the heel/face turns of Mongo and Lily.
First one that came to mind.
You’re disappointed somebody else didn’t beat you to it? You actually got to make a post and enlighten us with more on-topic treasures. I’d think anybody would cherish that opportunity.
The one that shined above all the rest was Victor Buono’s King Tut. A scenery-eater extraordinaire.
Dammit, I came here to mention Morty. The movie’s utterly forgettable early nineties cable-filler, but every scene with Tucci is comedy gold.
Brief hijack: I’m forcing myself to watch the entire run of the 60s Batman show and finding it horrible and painful in its incompetence. Until yesterday…when I got to “The Unkindest Tut of All” (Season 3, Episode 6) and to my utter surprise, I found myself laughing at clever dialogue (“What’s it all about, Alfred?”) and physical comedy that wasn’t ironic. Makes me feel a bit better about the possibilities for the rest of the season. (end hijack)
Also, re: the Catwoman debate. I like Hathaway’s costume the most of all of them, but Julie Newmar’s cheekbones turn me into a puddle every time she shows up onscreen, so she gets the edge as best Catwoman IHMO.
As I recall, Season 3 was truncated. I was very disappointed not to see the Joker’s flying saucer after it had been hyped in the tag to what turned out to be the last show in March 1968.
The first half-season (it debuted the first week of January 1966) was comic-booky but not egregously so (at least not to 11-year-old me, who took it dead seriously). It got really campy almost immediately in the second season, and by the start of the third I had lost interest in it. The show’s sagging production values mirrored its decline in the Nielsen ratings.
I have a huge crush on Hathaway too, but Julie and Lee top them all IMHO.
74 posts, and no mention of Sideshow Bob?
What, no mention of Jar Jar Binks!?!
That would be John Dehner, who played a pretty darn good comic villain in the Dabney Coleman mode in many roles, as well as a straight-up bad guy.
Do we count Roger C. Carmel as Harry Mudd in Star Trek as a comedy villain? Only his second appearance?
John Dehner is correct. Well done! 
Harry Mudd wasn’t exactly kosher in both episodes, or in the animated series either.
I like the Shame two-parter that’s on its way to you.
Is he a villain? More of a co-protagonist.