Since the 1940's Batman movie serials didn't use the villains from the comics, the 1960's show was the first time that Batman's iconic enemies were adapted.
Cesar Romero played the Joker in all three seasons of the show. He also appeared in the 1966 movie.
Burgess Meredith played the Penguin in all three seasons of the show. He also appeared in the 1966 movie and did audio recordings of the Penguin called The Capture and The Escape. He had a cameo as a character resembling the Penguin in an episode of The Monkees.
Julie Newmar played Catwoman in the first two seasons of the show. She appeared in the early 2000's Return to the Batcave: The Misadventures of Adam and Burt TV film. She voiced Catwoman in 2016's Batman: Return of the Caped Crusaders and 2017's Batman vs. Two-Face.
Lee Meriwether played Catwoman in the 1966 movie. She played Lisa Carson in the second season. She appeared in the early 2000's Return to the Batcave: The Misadventures of Adam and Burt TV film and voiced King Tut's lawyer in Batman vs. Two-Face.
Eartha Kitt played Catwoman in the third season.
Frank Gorshin played the Riddler in the first and third seasons. He also appeared in the 1966 movie and 1979's Legends of the Superheroes TV special. He also sang a Riddler song in the 1960's. He appeared in the early 2000's Return to the Batcave: The Misadventures of Adam and Burt TV film. He voiced Hugo Strange in three episodes of the 2000's The Batman cartoon series.
John Astin played the Riddler in the second season.
George Sanders played Mr. Freeze in the first season.
Otto Preminger was the first of two actors to play Mr. Freeze in the second season.
Eli Wallach was the second actor to play Mr. Freeze in the second season.
David Wayne played the Mad Hatter in the first two seasons.
Malachi Throne played False Face in the first season.
Walter Slezak played the Clock King in the second season.
Maurice Evans played the Puzzler (a character that's usually a Superman villain) in the second season.
Cesar Romero played the Joker in all three seasons of the show. He also appeared in the 1966 movie.
Burgess Meredith played the Penguin in all three seasons of the show. He also appeared in the 1966 movie and did audio recordings of the Penguin called The Capture and The Escape. He had a cameo as a character resembling the Penguin in an episode of The Monkees.
Julie Newmar played Catwoman in the first two seasons of the show. She appeared in the early 2000's Return to the Batcave: The Misadventures of Adam and Burt TV film. She voiced Catwoman in 2016's Batman: Return of the Caped Crusaders and 2017's Batman vs. Two-Face.
Lee Meriwether played Catwoman in the 1966 movie. She played Lisa Carson in the second season. She appeared in the early 2000's Return to the Batcave: The Misadventures of Adam and Burt TV film and voiced King Tut's lawyer in Batman vs. Two-Face.
Eartha Kitt played Catwoman in the third season.
Frank Gorshin played the Riddler in the first and third seasons. He also appeared in the 1966 movie and 1979's Legends of the Superheroes TV special. He also sang a Riddler song in the 1960's. He appeared in the early 2000's Return to the Batcave: The Misadventures of Adam and Burt TV film. He voiced Hugo Strange in three episodes of the 2000's The Batman cartoon series.
John Astin played the Riddler in the second season.
George Sanders played Mr. Freeze in the first season.
Otto Preminger was the first of two actors to play Mr. Freeze in the second season.
Eli Wallach was the second actor to play Mr. Freeze in the second season.
David Wayne played the Mad Hatter in the first two seasons.
Malachi Throne played False Face in the first season.
Walter Slezak played the Clock King in the second season.
Maurice Evans played the Puzzler (a character that's usually a Superman villain) in the second season.