The Triassic–Jurassic Upper Karoo Group of the Mid-Zambezi Basin (MZB; Zimbabwe) includes a thick succession of terrestrial sediments with high palaeontological potential that has been neglected since the 1970s. Here, we review the Upper Karoo Group stratigraphy, present detailed sedimentological work and identify new vertebrate-bearing sites at several measured sections along the southern shore of Lake Kariba. These fossil-bearing sites fall within the Pebbly Arkose and Forest Sandstone formations, and are the first to be recorded from the region since the discovery of Vulcanodon karibaensis nearly 50 years ago. The unique and diverse assemblage of aquatic and terrestrial fauna reported includes phytosaurs, metoposaurid amphibians, lungfish, non-dinosaurian archosauromorphs and non-sauropod sauropodomorph dinosaurs. This improvement of Upper Karoo Group biostratigraphy is important in refining its temporal resolution, and impacts both regional and global studies. Finally, the new fossil sites demonstrate the palaeontological importance of the MZB and its role in providing a holistic understanding of early Mesozoic ecosystems in southern Gondwana.