The Golden Mile and Mount Charlotte deposits in the Kalgoorlie Terrane, Western Australia, display three main mineralization styles: Fimiston, comprised of interconnected shear zones associated with ankerite-pyrite ± hematite- ± magnetite-gold-telluride alteration; Oroya, made up of breccia bodies with V-muscovite-ankerite-pyrite ± pyrrhotite-gold-telluride alteration; and Mount Charlotte, which consists of vein arrays with symmetrical ankerite-sericite-albite-pyrite ± pyrrhotite ± gold alteration. Pyrite is in equilibrium with gold in all three mineralization styles and has been selected as a proxy to record the sulfur source of the mineralizing fluids as well as the nature of the hydrothermal processes. The δ34S, Δ33S, and Δ36S analyses on pyrite grains from the different mineralization styles, including oxidized and reduced sulfide-oxide assemblages, reveal (1) a large variation in δ34S (from − 12.6 to + 23.5‰), and (2) a previously unrecognized occurrence of anomalous Δ33S and Δ36S signatures (from − 1.0 to + 1.1‰ and from − 2.3 to + 0.9‰, respectively). It is argued that the mineralizing fluids that formed the Golden Mile and Mount Charlotte deposits record mixing among three components: mantle sulfur, oxidized seawater sulfur (e.g., SO4), and reduced elemental sulfur (e.g., S8). Petrographic evidence in conjunction with Δ33S and Δ36S data suggest that MIF-S was acquired during the deposition of shales and basalts present in the Kalgoorlie Terrane and later mixed with mantle-derived sulfur during the mineralization events. The negative δ34S values that predominate in Fimiston style mineralization are consistent with a prevalence of oxidized fluids during the ore-forming process, as reflected by the presence of hematite-pyrite-magnetite-gold assemblages. Conversely, the positive δ34S values that dominate in the Mt Charlotte and Oroya mineralization styles reflect a reducing environment, as reflected by the presence of pyrite-pyrrhotite-gold assemblages.