http://www.toptenz.net/top-10-great-actors-who-made-awful-batman-villains.php

Aside from being a sublimely ridiculous TV series, Batman (the 1960’s version) was the prime destination for actors who would often be cast as villains. Enticed by the chance to ham it up and be a part of pop culture, serious actors such as Anne Baxter, Ida Lupino, Tallulah Bankhead, Victor Buono, Rudy Vallee, Burgess Meredith and Maurice Evans all appeared on the show.

Read more: http://www.toptenz.net/top-10-great-actors-who-made-awful-batman-villains.php#ixzz2SD181ysp

Agree with all except for David Wayne/The Mad Hatter. Walter Slezak/Clock King & Roddy McDowall/The Bookworm were much worse.

I remember famed hairdresser Jay Sebring guest starring but I don't know if he was a villian or not.

Rudy Vallee should have made the list.