Integrated structural, metamorphic, and geochronological data indicate that the evolution of the Southern Marginal Zone (SMZ) of the Limpopo Complex of southern Africa was controlled by a single Neoarchean high-grade tectono-metamorphic event. The exhumation history reflected by the high-grade rocks is determined by their location relative to the contact with the low-grade rocks of the Kaapvaal Craton. Exhumation of granulites far north from this contact is recorded by a decompression-cooling (DC) pressure-temperature (P-T) path linked to steep southward-verging thrusts related to the Hout River Shear Zone. This P-T path traverses from P ~8 kbar, T ~825 °C to P ~5 kbar, T ~550 °C and reflects exhumation of the SMZ in the interval ca. 2.68–2.64 Ga. P-T paths for granulites close to this contact are characterized by a distinct inflection at P ~6 kbar, T ~700 °C that exhibits near-isobaric cooling (IC) to T ~580 °C. The IC stage is linked to low-angle, out-of-sequence, southward-verging thrusts that developed in the interval 2.63–2.6 Ga. The thrust-controlled exhumation of the SMZ furthermore is demonstrated by the convergence at P ~6 kbar, T ~700 °C of DC P-T paths in the hanging wall with prograde P-T loops in the footwall of the steeply southward-verging Hout River Shear Zone, and by the establishment of a retrograde isograd and zone of rehydrated granulites in the hanging wall derived from the dehydration of the low-grade rocks in the footwall. A composite deformation-pressure-temperature-time (D-P-T-t) diagram provides evidence in support of a tectonic model for the evolution of the Limpopo Complex that involves early crustal thickening and peak metamorphic conditions followed by doming and diapirism related to gravitational redistribution mechanisms.