The Youjiang Basin in southwestern China hosts remarkably large amounts of Carlin-type Au deposits. In such deposits, Au is mainly ionically bound to arsenian pyrite characterized by core and rim textures. Understanding the formation mechanism of zoned pyrite may improve our understanding of the genesis of massive Carlin-type Au deposits. This study examined the elemental content, mineral composition, and pyrite texture and chemistry of wall rock and ore from the Lannigou Au deposit, one of the largest Carlin-type Au deposits in the Youjiang Basin, to identify the genetic mechanisms of zoned pyrite.Five distinct types of pyrites, i.e., pyrite 1 (Py1), 2 (Py2), 3 (Py3), 4 (Py4), and ore pyrite (OPy), were identified in the Lannigou Au deposit. Py1, Py2, and Py3 were mainly observed in the wall rock, whereas Py4 and OPy, constituting the core and rim of zoned pyrite, respectively, were only discovered in the ore. Mineral mapping of the wall rock and ore indicated that pyrite is scarce in the wall rock (0.021 vol%). However, the amount of zoned pyrite significantly increased in the ore (1.275 vol%). Py1, Py2, and Py3, showing framboidal, nodular, and fine euhedral microcrystal textures, had high Pb, Co, Ni, Mn, Zn, and Mo contents (medians ranging from 10 to 1,000 ppm) and variable δ34S compositions ranging from −5.1 to 35.4‰, implying a sedimentary (syngenetic or diagenetic) origin. Py4 was homogeneous and contained numerous illite and quartz inclusions and fractures. In contrast, OPy showed multiple As-rich sub-bands and a lack of illite or quartz inclusions and fractures. Py4 had significantly lower Au, As, Tl, and Cu contents than OPy; however, Py4 had Pb, Co, Ni, Mn, Zn, and Mo contents similar to OPy. The range of δ34S values for Py4 and OPy were both narrow, but Py4 (7.6 to 13.3‰, with an average of 9.1‰) had lower δ34S values than OPy (9.4–14.1‰, with an average of 12.4‰). These texture and chemical features indicate that Py4 likely sedimented from a pre-ore hydrothermal fluid, but not at the early stage of the ore-forming fluid.Hydrothermal pyrite cores were also widespread and exhibited textural and chemical differences compared to Au-rich pyrite rims from other Au deposits in the Youjiang Basin. Based on the two geochronological clusters of Au deposits in the Youjiang Basin, we inferred the occurrence of at least two episodes of large-scale hydrothermal events. The two hydrothermal fluid episodes, which contributed to the zoned pyrite formation, likely originated from the mixing of initial magmatic fluid with δ34S values of ∼0 ± 5‰ and basin brine with elevated δ34S values (δ34S > 18‰). Pre-ore hydrothermal pyrite likely resulted in the rapid non-equilibrium crystallization of ore pyrite; thus, more Carlin-suite elements were captured by ore pyrite. Additionally, low-grade Au orebodies may have locally formed during the pre-ore hydrothermal event. These multiple hydrothermal events may have been crucial for the formation of massive Carlin-type Au deposits in the Youjiang Basin.