It's off-topic here, because the comic is from 1948, but I couldn't resist writing about this one. There have been plenty of bizarre villains in the history of comic books, but you're going to have to work hard to beat this guy:
Meet Pinball. As has been traditional in comics for ages, his head resembles his namesake--see the Vulture, the Clock and the Shark for some other examples. His schtick consists of sending wealthy men pinball machines with some theme that will amuse them--cars for an auto racing magnate, jewels for a jeweler, etc. Of course, the machines are gimmicked to somehow incapacitate the recipient so Pinball and his minions can rob him at their leisure.
The Star Spangled Kid encounters him when his dad (a wealthy banker) receives a machine. As is also traditional in these stories, when the villain is captured the hero must close the tale with a pun on the theme: