The Natal Group and Msikaba Formation remain relatively poorly understood with regards to their provenance and relative age of deposition; a much-needed geochronological study of the detrital zircons from these two units was therefore undertaken. Five samples of the Durban and Mariannhill Formations (Natal Group) and the Msikaba Formation (Cape Supergroup) were obtained. A total of 882 concordant U–Pb ages of detrital zircon populations from these units were determined by means of laser ablation inductively coupled plasma mass spectrometry (LA-ICP-MS). Major Neoproterozoic and secondary Mesoproterozoic detrital zircon age populations are present in the detrital zircon content of all the samples. Smaller contributions from Archean-, Palaeoproterozoic-, Cambrian- and Ordovician-aged grains are also present. Due to the presence of a prominent major population of 800–1000 Ma zircons in all the samples, late Stenian – Tonian ancient volcanic arc complexes overprinted by Pan-African metamorphism of Mozambique, Malawi and Zambia, along with areas of similar age within Antarctica, India and Sri Lanka, are suggested as major sources of detritus. The Namaqua–Natal Metamorphic Complex is suggested as a possible source of minor late Mesoproterozoic-aged detritus. Minor populations of Archean and Palaeoproterozoic zircons were likely sourced from the Kaapvaal and Grunehogna Cratons. Post-orogenic Cambrian – Lower Ordovician granitoids of the Mozambique Belt (Mozambique) and the Maud Belt (Antarctica) made lesser contributions. In view of the apparent broad similarity of source areas for the Natal Group and Msikaba Formation, their sedimentation occurred in parts of the same large and evolving basin rather than localized in small continental basins, and the current exposures merely represent small erosional relicts.