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Enhancing charge separation in semiconductor photocatalysts is a major challenge for efficient artificial photosynthesis. Herein, a compact heterojunction is designed by embedding half‐metallic C(CN)3 (hm‐CN) hydrothermally in BiOBr (BOB) as the backbone. The interface between hm‐CN and BOB is seamless and formed by covalent bonding to facilitate the transmission of photoinduced electrons from BOB to hm‐CN. The transient photocurrents and electrochemical impedance spectra reveal that the modified composite catalyst exhibits a larger electron transfer rate. The photocatalytic activity of hm‐CN/BOB increases significantly as indicated by a CO yield that is about four times higher than that of individual components. Density‐functional theory calculations verify that the heterojunction improves electron transport and decreases the reaction energy barrier, thus promoting the overall photocatalytic CO2 conversion efficiency. The half‐metal nitride coupled semiconductor heterojunctions might have large potential in artificial photosynthesis and related applications. [ABSTRACT FROM AUTHOR]

A S-Scheme heterojunction with close contact between CN and CoTPP was establish by a unique synthesis method. Formation of S-type heterojunction facilitated the efficient separation of photogenerated carriers and improved photocatalytic activity. [Display omitted] • The g-C 3 N 4 is rapidly synthesized by the technology of thermal polycondensation. • Co-porphyrins is introduced to increase the catalytic activity of the catalyst. • Adjusting the ratio of loads can regulate the activity of CO 2 reduction. • S-scheme heterojunction promotes efficient separation of photogenerated carriers. The emissions of CO 2 are increasing year by year, which have led to serious environmental problems. Converting CO 2 into valuable fuels through photocatalysis is a promising strategy. In this research, oxygen atoms were successfully innovated into graphitic carbon nitride (CN). Additionally, cobalt porphyrin (CoTPP) was successfully loaded onto the modified carbon nitride (Co/CN). The generation of interfacial electric fields and bending bands between CN and CoTPP was demonstrated experimentally. The electrons in the CN and the holes in the CoTPP were combined to form a unique S-scheme heterojunction structure, and efficient separation of carriers was promoted. As a result, the CO conversion under visible light irradiation reached an impressive 100.70 μmol g−1 h−1. By integrating theoretical and experimental findings, this study underscores the critical role of catalyst design in enabling efficient photocatalytic CO 2 reduction. [ABSTRACT FROM AUTHOR]