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A well-designed cocatalyst structure can improve the light-harvesting and quantum efficiency of photocatalysis. A multidimensional MoO2-C@MoS2 (MOCS) cocatalyst was successfully synthesized by post-sulfidation of MoO2-C nanorods. This controlled sulfidation process effectively inhibits the undesired oxidation of MoO2, stabilizing its metallicity and creating a synergistic effect for H2 evolution. Firstly, the highly dispersed metallic MoO2 nanoparticles induce localized surface plasmon resonance effects, expanding the light-harvesting range and generating abundant hot electrons. Secondly, the build-in electrostatic field and highly conductive carbon framework facilitates efficient interfacial electrons transfer. Thirdly, the amorphous MoOx and fragmented few-layers MoS2 in MOCS provide dual active sites with superior intrinsic activity for H2 evolution. Moreover, the unique multi-interface structure of MOCS optimizes the separation and reaction of charge carriers. As a result, the 20 wt% MOCS/CdS system show an excellent quasi-full-spectrum driven photocatalytic H2 evolution activity of 48.41 mmol/h·g, with 4.03 mmol/h·g in near-infrared region (> 800 nm).
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•Multidimensional MoO2-C@MoS2 cocatalyst enhances quasi-full-spectrum photocatalytic H2 evolution performance of CdS.•Controlled sulfurization inhibits MoO2 oxidation and creates a synergistic effect with formed MoS2 nanosheets.•Highly dispersed metallic MoO2 induces LSPR effect, expanding light harvest range to near-infrared region.•MoOx and fragmented few-layers MoS2 provide numerous active sites with superior intrinsic activity for HER.•The multi-interface structure of cocatalyst optimizes photogenerated carriers’ efficiency in photocatalysis.