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[Display omitted] • The UCN@ZIS/SWNTs composite with different V Zn concentrations was constructed for photocatalytic CO 2 reduction. • The UCN was acidified to regulate the surface-active site for CO 2 activation and H 2 O dissociation. • The SWNTs further improves the separation efficiency of photogenerated electron-hole pairs by providing charge transfer channels. • The UCN@rZIS/SWNTs composite displays excellent photocatalytic performance and CH 4 selectivity. Zinc vacancy (V Zn) concentrations were successfully regulated on the hierarchical flower spherical ZnIn 2 S 4 (ZIS) by controlling the hydrothermal temperature. The photo-electrochemical experiments indicated that the carrier separation efficiency of ultrathin-g-C 3 N 4 @ZIS/SWNTs (UCN@ZIS/SWNTs) composite with different V Zn concentrations (poor-V Zn ZIS (pZIS) and rich-V Zn ZIS (rZIS)) had an efficient improvement because of the construction of UCN@ZIS heterojunction and the multiple channels for charge transfer provided by SWNTs. In-situ FTIR results indicate that the presence of V Zn and the enriched surface-active site on UCN contributes to CO 2 activation and H 2 O dissociation. Additionally, the yield of CO and CH 4 over UCN@rZIS/SWNTs composite reached 33.7 µmol g−1 and 39.8 µmol g−1, respectively, and the selectivity of CH 4 reached 54.1 % under the synergistic effect of V Zn , the surface-active site of UCN and charge-transfer channels. This work established an ideal defect model for enhancing CO 2 photocatalytic reduction performance and product selectivity, which may provide a new way to improve photocatalytic efficiency and a better understanding of the photocatalytic reaction mechanisms. [ABSTRACT FROM AUTHOR]