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Visible light-driven C–C bond formation has attracted increasing attention recently, thanks to the advance in molecular photosensitizers and organometallic catalysts. Nevertheless, these homogeneous methodologies typically necessitate the utilization of noble metal-based (e.g., Ir, Ru, etc.) photosensitizers. In contrast, solid-state semiconductors represent an attractive alternative but remain less explored for C–C bond-forming reactions driven by visible-light irradiation. Herein, we report that photocatalytic pinacol C–C coupling of benzaldehyde to hydrobenzoin can be achieved on two-dimensional ZnIn₂S₄ nanosheets upon visible-light irradiation in the presence of a sacrificial electron donor (e.g., triethylamine). We further demonstrate that it is feasible to take advantage of both excited electrons and holes in irradiated ZnIn₂S₄ for C–C coupling reactions in the absence of any sacrificial reagent if benzyl alcohol is …