According to
http://batman.wikia.com/wiki/Villain..._(1960s_series)
the Villains created for the series are
King Tut (Victor Buono)
Egghead (Vincent Price)
The Bookworm (Roddy McDowall)
Shame (Cliff Robertson)
Ma Parker (Shelley Winters)
Marsha, Queen of Diamonds (Carolyn Jones)
The Sandman (Michael Rennie)
Black Widow (Tallulah Bankhead)
Siren (Joan Collins)
Colonel Gumm (Roger C. Carmel)
Chandell (Liberace) & Harry (Liberace)
Zelda the Great (Anne Baxter)
Minerva (Zsa Zsa Gabor)
The Minstrel (Van Johnson)
Lord Marmaduke Ffogg (Rudy Vallee)
Louie the Lilac (Milton Berle)
Dr.Cassandra Spellcraft (Ida Lupino)
Nora Clavicle (Barbara Rush)
Olga, Queen of Cossacks (Anne Baxter)
Freddy the Fence (Jacques Bergerac)
Lola Lasagne (Ethel Merman)
Lady Penelope Peasoup (Glynis Johns)
Calamity Jan (Dina Merrill)
Cabala (Howard Duff)
