The gold-bearing arsenian pyrite in Carlin-type gold deposits typically grows around the gold/arsenic-poor pyrite core, forming core–rim textured pyrite. However, the causes of rim pyrite precipitation around the early-formed core pyrite and the growth mechanisms of the rim pyrite remain unclear. Here, we combined scanning electron microscopy, electron probe micro-analysis, and nanoscale secondary ion mass spectrometry to investigate the textural and chemical characteristics of core–rim textured pyrite from the giant Shuiyindong and Lannigou gold deposits. Furthermore, we used electron backscattered diffraction and transmission electron microscopy to characterize their crystallographic structure. The results indicated that core–rim textured pyrite is the dominant pyrite type in the ore. This type of pyrite is characterized by the sharp core–rim interfaces, euhedral-subhedral morphology, and oscillating zoning. The gold/arsenic-rich rim and gold/arsenic-poor core formed during the main-ore and pre-ore stages, respectively. Crystallographically, the rim showed that a crystallographic orientation is similar to that of the core along the (0 1 0) crystal facet, indicating that the core pyrite serves as a template for the epitaxial growth of rim pyrite. Textural and chemical features indicate that the epitaxy occurs in the process of direct precipitation of main-ore pyrite over the pre-ore pyrite. As Carlin ore fluids dissolve the iron-bearing carbonates, iron concentrations in the fluids increase, thereby creating a supersaturation environment suitable for the nucleation of main-ore pyrite. Because the minimal lattice misfit would minimize the surface free energy and the (0 1 0) facet of pyrite has a lower surface energy than other facets, the nucleated pyrite would readily grow along the (0 1 0) facet of preexisting pyrite via epitaxy. Our findings highlight that the widespread preexisting pyrite facilitates late-stage pyrite precipitation. For Carlin-type gold deposits, the pre-ore pyrite is essential owing to its promoting the precipitation of gold-bearing pyrite.