A comparison of high-alumina mineral assemblages spatially associated with the Haile and Brewer gold deposits in the Paleozoic Carolina slate belt (CSB) of the southeast United States and the Sons of Gwalia and Mount Celia gold deposits in the Archean Norseman–Wiluna greenstone belt (NWGB) in Western Australia suggests a similar hydrothermal origin and subsequent metamorphic and deformational history. A common hydrothermal origin is supported by the striking similarity in whole-rock chemistry, even though there were probably significant variations in original unaltered protoliths. An analysis of rocks from each of the deposits that contain high-alumina minerals demonstrates that the protoliths were leached of alkalis with respect to aluminum and have a ratio of Al2O3/Na2O + CaO + K2O greater than three. Although the rocks contain abundant high-alumina minerals, the aluminum content in these rocks is not unusually high, and it does not appear that there has been any significant transport of aluminum either into or out of the rocks that were altered.The most common high-alumina minerals found in rocks affected by the feldspar destructive alteration event include andalusite, kyanite, pyrophyllite, kaolinite, and sericite. Other minerals present in variable amounts include diaspore, chloritoid, alunite, natroalunite, paragonite, and topaz. It is possible that some of these minerals formed during the early hydrothermal alteration event and were recrystallized during metamorphism. Regardless of when the high-alumina minerals formed, textural relations suggest that the rocks had been hydrothermally altered by the time the metamorphic minerals formed. A comparison of alteration from the deposits studied in the CSB and the NWGB suggests there are many similarities to acid-sulfate alteration associated with geothermal areas, such as Yellowstone Park, Wyoming, and with acid-sulfate gold deposits, such as Goldfield, Nevada. Thus, it is possible that the protolith of the metamorphosed rocks in the CSB and NWGB contained an alteration assemblage that included alunite, pyrophyllite, and kaolinite.A generalized paragenetic sequence determined from petrographic and field observations, beginning with regional metamorphism, follows: (i) formation of andalusite, kyanite, chloritoid, and topaz during prograde metamorphism, depending on whole rock chemistry, (ii) formation of pyrophyllite and quartz-rich pods during silicification of aluminosilicate-bearing rocks, (iii) bedding parallel schistosity and fracturing produced by a deformational event, (iv) fractures filled by quartz, sericite, pyrophyllite, or calcite, (v) folding of early layering in the rocks to form a crenulation cleavage accompanied by introduction of quartz veins at high angles to foliation; and (vi) retrograde metamorphism of andalusite–kyanite-pyrophyllite to produce an assemblage of kaolinite ± diaspore.The spatial association of the acid-sulfate alteration with gold mineralization, together with comparison of analogous alteration associated with younger unmetamorphosed acid-sulfate gold deposits, suggests that at least some of the gold was introduced during the early premetamorphic alteration event. The present location of gold in each deposit is a result of local changes brought about by later metamorphic and deformational events.