The Archean-Proterozoic transition marks a time of fundamental geologic, biologic, and atmospheric changes to the Earth system, including oxygenation of the atmosphere (termed the Great Oxygenation Event; GOE), and the emergence of continents above sea-level. The impacts of the GOE on Earth’s surface environment are imprinted on the geologic record, including the attenuation of mass-independent fractionation of sulfur isotopes (S-MIF). Temporally overlapping geologic and geochemical observations (e.g. a change in oxygen isotope ratio of sediment melts) imply the widespread subaerial emergence of continents was coeval with atmospheric oxygenation. Here we present triple sulfur isotope ratios in pyrite and oxygen isotope ratios in garnet and zircon in a global suite of Archean and Proterozoic sediment-derived granitoids. These crustal melts record an increase in average 18O/16O isotope ratio and a disappearance of S-MIF in the Paleoproterozoic. The coupled behaviour of sulfur and oxygen isotope signatures imply a potential causal link between the emergence of continents and atmospheric oxygenation at ~2.3 Ga.