Comics fans know the Mole Man is more closely associated with the Fantastic Four. However, he beat the FF to television by one year, when The Marvel Superheroes Show adapted his battle with Iron Man from an issue of Tales of Suspense. Unfortunately, the producers erred by spelling the villain's name as one word.
Uploaded by The Armor Gallery.
Yes, the Mole Man would eventually appear on the FF's show the next year, but insofar as I know, he never menaced Iron Man again.