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An interfacial C-S bond bridged ZnS/C 3 N 5 S-scheme heterojunction was constructed for photocatalytic H 2 evolution. Benefiting from the interfacial covalent bond, enhanced internal-electric-field strength, and accelerated surface photocatalytic reaction, the photocatalytic H 2 production of ZnS/C 3 N 5 was 3.2 and 2.5 times higher than those of ZnS/C 3 N 4 and ZnS/C 3 N 5 -300 without C-S bond. [Display omitted] • C-S bond is susceptive to preparation temperatures, and it is broken above 300 °C. • C-S bond promotes e − separation and improves H 2 O adsorption and activation behaviors. • IEF strength of ZnS/C 3 N 5 with opposite direction is 2.6 times than that of ZnS/C 3 N 4. • e − transfer respectively follow S-scheme and type-II pathway in ZnS/C 3 N 5 and ZnS/C 3 N 4. • H 2 yield of ZnS/C 3 N 5 is 3.2 and 2.5 times than ZnS/C 3 N 4 and ZnS/C 3 N 5 -300 without C-S. An interfacial C-S bond bridged ZnS/C 3 N 5 heterojunction was constructed for photocatalytic H 2 evolution. Different from traditional type-II ZnS/C 3 N 4 heterojunction, the electron transfer followed S-scheme pathway, due to opposite internal-electric-field (IEF) directions in these two heterojunctions. The C-S bond formation was carefully investigated, and they were susceptive to the preparation temperatures. In photocatalytic reaction, C-S bond was functioned as the "high-speed channel" for electron separation and transfer, and the IEF strength in ZnS/C 3 N 5 was 1.86 × 108 V/m, 2.6 times higher than that in ZnS/C 3 N 4. Moreover, the C-S bond also altered the surface molecular structure of ZnS/C 3 N 5 , and hence the surface reaction was accelerated via improving H 2 O adsorption and activation behaviors. Benefiting from the S-scheme pathway, enhanced IEF strength, and accelerated surface reaction, the photocatalytic H 2 production over ZnS/C 3 N 5 reached up to 20.18 mmol/g/h, 3.2 and 2.5 times higher than those of ZnS/C 3 N 4 and ZnS/C 3 N 5 -300 without C-S bond. [ABSTRACT FROM AUTHOR]