Along the >650 km long southern margin of the Karoo Basin in South Africa, we traversed four evenly spaced stratigraphic transects and collected 22 samples of volcanic, air-fall tuffs thought to be distal deposits derived from the Permian–Triassic Southern Gondwanan volcanic arc. We present 469 new U-Pb zircon ages determined by sensitive high-resolution ion microprobe reverse geometry (SHRIMP-RG) at the Stanford–USGS Microanalytical Center in order to constrain the maximum depositional ages for the southern Karoo Basin strata. Weighted means of these youngest coherent zircon populations were selected to maximize the number of analyses while minimizing the mean square weighted deviation (MSWD) to increase the robustness and decrease the influence of Pb-loss and inheritance in determining the maximum depositional age. Maximum depositional ages for the marine Ecca Group range from 250 to 274 Ma, whereas in the conformably overlying terrestrial Beaufort Group maximum depositional ages ranged from 257 to 452 Ma. Across the southern Karoo Basin, the Ecca Group tuffs produce maximum depositional ages that young upward; however, the Beaufort Group tuffs yield maximum depositional ages that are geochronologically out of sequence. Furthermore, maximum depositional ages of the Beaufort Group tuffs are consistently older than ash ages within the underlying marine strata. Our results are supported by previously published U-Pb tuff zircon geochronology in the Karoo Basin and demonstrate that the presence of out-of-sequence, older tuff ages are repeatable in Beaufort Group tuffs along the southern margin of the basin. We propose that tuffs in the Karoo Basin are correlative with tuffs in southern South America, and that the age spectra of these tuffs were influenced by magmatic crustal recycling. We use these data to highlight the complexity of U-Pb zircon datasets from tuffs, address the use of U-Pb zircon ages to provide absolute age controls, and discuss the implications of these new age controls on the Permian-Triassic Karoo strata.