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The demise of the Late Paleozoic Ice Age has been hypothesized as diachronous, occurring first in western South America and progressing eastward across Africa and culminating in Australia over an ~60 m.y. period, suggesting tectonic forcing mechanisms that operate on time scales of 106 yr or longer. We test this diachronous deglaciation hypothesis for southwestern and south-central Gondwana with new single crystal U-Pb zircon chemical abrasion thermal ionizing mass spectrometry (CA-TIMS) ages from volcaniclastic deposits in the Paraná (Brazil) and Karoo (South Africa) Basins that span the terminal deglaciation through the early postglacial period. Intrabasinal stratigraphic correlations permitted by the new high-resolution radioisotope ages indicate that deglaciation across the south to southeast Paraná Basin was synchronous, with glaciation constrained to the Carboniferous. Cross-basin correlation reveals two additional glacial-deglacial cycles in the Karoo Basin after the terminal deglaciation in the Paraná Basin. South African glaciations were penecontemporaneous (within U-Pb age uncertainties) with third-order sequence boundaries (i.e., inferred base-level falls) in the Paraná Basin. Synchroneity between early Permian glacial-deglacial events in southwestern to south-central Gondwana and pCO2 fluctuations suggest a primary CO2 control on ice thresholds. The occurrence of renewed glaciation in the Karoo Basin, after terminal deglaciation in the Paraná Basin, reflects the secondary influences of regional paleogeography, topography, and moisture sources.