Several new specimens of the Triassic therocephalian Tetracynodon darti have become available in recent years, allowing substantial corrections and expansions to previous descriptions. We here analyze T. darti in the context of therocephalian relationships and biology, using computed tomographic (CT) scanning to reveal details of the skull. Histological sections, as well as the degree of ossification of individual elements, both suggest that the available specimens are subadults (rather than rapidly growing neonates), and probably yearlings. A maxillary shelf bearing a long suture with the vomer similar to that of Lycideops is present, and T. darti also shares a nasal-lacrimal contact with that taxon. There is no evidence for the presence of maxilloturbinal bones. The postcranial skeleton is slender and similar to that of regisaurids and other small baurioids. The skull bones show clear indentations demarcating the major divisions of the brain, allowing one of the most detailed reconstructions of a non-mammalian therapsid brain published to date. The brain is strikingly plesiomorphic in many features, particularly in the retention of large dorsally positioned optic lobes of the tectum, but generally shows features that are intermediate between gorgonopsians and cynodonts, thus clarifying this stage of the evolution of the synapsid brain. A cladistic analysis of 33 therapsid taxa and 131 morphological characters supports the monophyly of Therocephalia, and there is evidence for a monophyletic Lycideopidae within Baurioidea. Lycideopidae contains species with long snouts, nasal-lacrimal contacts, and incipient secondary palates, including Lycideops, Choerosaurus, T. tenuis, and T. darti.