The Gondwanatheria are an enigmatic clade of Cretaceous and Paleogene mammals known from South America, Africa, Madagascar, India, and the Antarctic Peninsula. The eight valid species—each belonging to a monotypic genus and the first of which was described only 30 years ago—are represented almost exclusively by isolated teeth, in addition to fragmentary dentaries attributed to Sudamerica, Gondwanatherium, Ferugliotherium, and an unnamed taxon from Tanzania. No cranial (skull exclusive of lower jaw) or postcranial material has heretofore been assigned to the Gondwanatheria, a severe limitation that has precluded a comprehensive assessment of phylogenetic affinities. Here we describe, in detail, the first cranial specimen of a gondwanatherian mammal. This material consists of a complete and wellpreserved cranium of the sudamericid Vintana sertichi, recovered from the Upper Cretaceous (Maastrichtian) Maevarano Formation in the Mahajanga Basin of northwestern Madagascar. Salient features of the cranium include elongate, scimitarlike jugal flanges, huge orbits, strong klinorhynchy, and a vaulted nuchal region. Micro-computed tomography greatly facilitated the delineation of sutures and the description of internal morphology. The cranial features of Vintana are compared with those of a broad range of synapsids, with particular concentration on other Mesozoic mammaliaforms. The cranium of Vintana exhibits a mosaic of extremely primitive and extremely derived features. It is the second largest known for a Mesozoic mammaliaform, superseded only by that of the eutriconodontan Repenomamus giganticus from the Early Cretaceous of China. Vintana is the largest known Late Cretaceous mammaliaform; it is also the largest known Mesozoic mammaliaform from Gondwana.