I recall Gould saying in an interview he made his villain so grotesque because it reflected their inner ugliness. Personally, I think all his characters are funny-looking, from Junior to Sparkle Plenty to Sam but that was his style.
Someone should do a big graphic novel where Golden Age Batman goes to the Dick Tracy universe and tackles the Brow, Flattop, Pruneface, the Blank and all the rest. They might like fighting a hero who wants to take them in alive.