The elemental accumulation and recycling in the metamorphosed Keketale VMS-type Pb-Zn deposit of the Altai Mountains are presented in this study. Based on detailed fieldwork and microscopic observation, the formation of the deposit involved syngenetic massive sulfide mineralization and epigenetic superimposed mineralization. Different generations of iron sulfides (i.e., pyrite and pyrrhotite) with contrasting textural, elemental, and sulfur isotopic features were generated in primary mineralization (including hydrothermal iron sulfides, colloform pyrite) and secondary modification (including annealed iron sulfides, oriented iron sulfides, and vein-pyrite). It is revealed that the spatial variation in textures and elements of hydrothermal iron sulfides depends on the inhomogeneous fluid compositions and varied environment in VMS hydrothermal system. Both leached sulfur from the footwall volcanic rocks and reduced sulfur by the TSR process are regarded as important sulfur sources. Furthermore, large sulfur isotopic fractionation and negative δ34S values were mainly caused by varied oxygen fugacity, and to a lesser extent, temperature fluctuation. The epigenetic polymetallic veins that contain sulfides and sulfosalts (e.g., jordanite-geocronite, bournonite-seligmannite, boulangerite) were considered as the products of metamorphic fluid scavenged the metal-rich strata. All things considered, it is indicated that two episodes of fluid with distinct origins were essential for the formation of the deposit. The predominant evolved seawater along with subordinate magmatic fluid mobilized metals from volcanic rocks and precipitated massive sulfides near the seafloor are vital for primary mineralization. The metamorphic fluid remobilized metals (i.e., FMEs: fluid mobile elements, e.g., Pb, As, Sb) from neighboring volcanic and pyroclastic rocks and destabilized them within the fractured zone are responsible for secondary mineralization, which enhances the economic value of the deposit. Accordingly, metal-rich Devonian strata had been successively swept by different origins of fluid, leading to progressively elemental enrichment and the formation of a large deposit. Furthermore, the current study enlightens that FME-bearing veins with economic benefits can be discovered near the metamorphosed VMS deposits.