Carlin-type gold deposits are one of the most important gold mineralization styles in the world. Despite their economic importance and the large volume of work that has been published, there remain crucial questions regarding their metallogenesis. Much of this uncertainty is due to the cryptic nature of the gold occurrence, with gold occurring as dispersed nanoscale inclusions within host pyrite rims that formed on earlier formed barren pyrite cores. The small size of the gold inclusions has made determining their nature within the host sulfides and the mechanisms by which they precipitated from the ore fluids particularly problematic. This study combines high-resolution electron probe microanalysis (EPMA) with atom probe tomography (APT) to constrain whether the gold occurs as nanospheres or is dispersed within the Carlin pyrites. APT offers the unique capability of obtaining major, minor, trace, and isotopic chemical information at near-atomic spatial resolution. We use this capability to investigate the atomic-scale distribution of trace elements within Carlin-type pyrite rims, as well as the relative differences of sulfur isotopes within the rim and core of gold-hosting pyrite.