The Araçuaí Orogen, in eastern Brazil, was formed during the Neoproterozoic – Cambrian amalgamation of West Gondwana. During the Mesozoic – Cenozoic opening of the South Atlantic Ocean, and the associated divergent tectonics, the orogen developed as basement to the passive margin of South America and was progressively covered by thick offshore sedimentary basins, particularly the Espírito Santo, Mucuri, and Cumuruxatiba basins, in which hydrocarbon systems have been exploited. Our understanding of the Araçuaí Orogen's passive margin evolution, erosion, and sediment transfer to these basins ultimately depends on constraining the onshore exhumation in response to Mesozoic – Cenozoic events. Here, new and previously published data from apatite fission-track (AFT) analyses and inverse thermal history modelling of (Pre)Cambrian basement rocks from the Araçuaí Orogen resolve three discrete basement cooling and associated erosional exhumation episodes. In the Pre-Rift phase, Jurassic – Hauterivian erosion of the Araçuaí Orogen is most likely related to the adjoining intra-continental West Gondwana flexural subsidence, which increased hillslope and river erosion power. In the Rift and Transitional phases, Barremian – Albian accelerated phase of erosion is associated with the uplift of the Atlantic rift shoulders and the establishment of an oceanic base-level. In the Drift phase, reactivations in response to far-field stresses likely triggered a Late Cretaceous – Paleocene rapid erosion event. The rates at which these events unfolded vary spatially and are controlled by inherited structures. The Araçuaí Orogen experienced slower denudation rates in areas closer to the São Francisco Craton, which suggests that the tectonic reactivation and related surface uplift during the Mesozoic–Cenozoic is in first-order controlled by lithospheric rigidity. Furthermore, the structural framework of the Paramirim and Pirapora aulacogens and NE-oriented shear zones in the orogen’s southeast facilitated later reactivations. From the spatial pattern of denudation/exhumation of the Araçuaí Orogen during the Mesozoic – Cenozoic, we draw inferences on the tectonic development of the offshore basins regarding their hydrocarbon potentials.