Siliciclastic rocks of the upper Byrd Group in the Transantarctic Mountains record rapid denudation and molasse deposition during Ross orogenesis along the early Paleozoic convergent margin of Gondwana. These rocks, which stratigraphically overlie Lower Cambrian Byrd carbonate deposits, are dominated by fresh detritus from proximal igneous and metamorphic sources within the Ross Orogen. Biostratigraphic evidence indicates that deposition of the siliciclastic succession is late Botomian or younger (<515 Ma). The largest modes of U-Pb and 40 Ar/ 39 Ar ages from detrital zircons and muscovites respectively in the siliciclastic molasse are Early to Middle Cambrian, but based on ages from crosscutting igneous bodies and neoblastic metamorphic phases, deposition of individual molasse units continued until ∼490–485 Ma (earliest Ordovician). The entire episode of interrelated tectonic, denudational, sedimentary, deformational, and magmatic events is restricted to a time interval of 7–25 m.y. in the late Early Cambrian to earliest Ordovician, within the resolution of these stratigraphic and geochronologic data. Stratigraphic relationships suggest that the detrital zircon and muscovite in the sediments came from the same source terrain, consistent with large volumes of molasse having been shed into forearc and/or marginal basins at this time, primarily due to erosion of igneous rocks and metamorphic basement of the early Ross magmatic arc. Rapid erosion and unroofing in the axial Ross Orogen is consistent with a sharp carbonate-to-clastic stratigraphic transition observed in the upper Byrd Group, reflecting an outpouring of alluvial fan and fluvial-marine clastic detritus. The short time lag between tectonism and sedimentary response is similar to that determined for the corresponding section of the Ross-Delamerian orogen in South Australia and other continental-margin arc systems, such as in the Mesozoic Peninsular Ranges of California. Mineral cooling ages from metamorphic basement adjacent to the orogen yield a syn- to late-orogenic cooling rate of ∼10 °C/m.y., which, combined with a known metamorphic geotherm, indicates a denudation rate of ∼0.5 mm/yr. Such denudation rates are comparable to those in recent convergent or collision orogens and suggest that crustal thickening associated with both magmatic intrusion and structural shortening was balanced by near-synchronous erosional exhumation.