Sclerocephalus was often classified within the deprecated paraphyletic taxa Stegocephalia and Labyrinthodontia, because of a skull that was connected to the shoulder girdle and teeth of labyrinthodont type.

From specimens with fossilized stomach content we know the adults mainly fed on fish of the genus Paramblypterus, but sometimes also on other amphibians (Branchiosaurus, Micromelerpeton) and even small conspecifics.

The famous American vertebrate paleontologist Alfred Romer recognized in 1939 that the fossil amphibians described as Leptorophus levis are the larvae of Sclerocephalus.

A famous locality that yielded numerous excellently preserved fossils of Sclerocephalus is Odernheim am Glan in Rhineland-Palatinate (Germany), where the Permian sediments of the Rotliegend have even been named "Stegocephalenkalke" (= Stegocephalia limestones).

[1] The most commonly accepted phylogeny of temnospondyls (first proposed by Yates and Warren [2000]) divides the group into two different branches called Limnarchia and Euskelia.

[2] An earlier phylogeny proposed by Boy (1990) takes a different view, combining Eryopidae and Stereospondylomorpha into the group Eryopoidea, with dissorophoids as distant relatives.