A recurring trend in Batman shows is to primarily use Batman's main enemies, while throwing in a few new villains. The 60s' Batman show created several of their own villains.

Villains That Were Originally From The Comics:

The Joker (In most versions of Batman, the Joker is Batman's main enemy. However, in the 60's show, he and Penguin had the same amount of appearances. Also, Penguin was the one who called the shots in the 60s' movie.)

The Penguin

Catwoman

The Riddler (Riddler was actually a minor Batman villain in the comics. Thanks to how great the Riddler was in the 60s' show, he's become one...