A study on the in-situ surface reconstruction of two-dimensional CdPS₃ nanosheets for efficient biomass hydrogenation is presented. The research demonstrates that the in-situ formation of a CdS layer on CdPS₃ nanosheets creates a CdPS₃/CdS heterostructure, which enhances the catalytic activity for the hydrogenation of 5-hydroxymethylfurfural (HMF) to 2,5-bis(hydroxymethyl)furan (BHMF). The catalyst achieves a Faradaic efficiency of 91.3 ± 2.3% and a yield of 4.96 ± 0.16 mg/h at -0.7 V versus reversible hydrogen electrode. Density functional theory (DFT) calculations show that the CdS layer optimizes the adsorption of HMF* and H* intermediates, facilitating the hydrogenation process. When combined with a MnCo₂O₄.5 anode, the CdPS₃/CdS cathode enables the simultaneous synthesis of BHMF and formate from HMF and glycerol substrates under ambient conditions. The study highlights the importance of surface reconstruction in enhancing catalytic performance and provides insights into the structure-activity relationship for efficient biomass conversion. The findings suggest that the CdPS₃/CdS heterostructure is a promising catalyst for hydrogenation reactions, offering a sustainable alternative to traditional thermocatalytic methods.A study on the in-situ surface reconstruction of two-dimensional CdPS₃ nanosheets for efficient biomass hydrogenation is presented. The research demonstrates that the in-situ formation of a CdS layer on CdPS₃ nanosheets creates a CdPS₃/CdS heterostructure, which enhances the catalytic activity for the hydrogenation of 5-hydroxymethylfurfural (HMF) to 2,5-bis(hydroxymethyl)furan (BHMF). The catalyst achieves a Faradaic efficiency of 91.3 ± 2.3% and a yield of 4.96 ± 0.16 mg/h at -0.7 V versus reversible hydrogen electrode. Density functional theory (DFT) calculations show that the CdS layer optimizes the adsorption of HMF* and H* intermediates, facilitating the hydrogenation process. When combined with a MnCo₂O₄.5 anode, the CdPS₃/CdS cathode enables the simultaneous synthesis of BHMF and formate from HMF and glycerol substrates under ambient conditions. The study highlights the importance of surface reconstruction in enhancing catalytic performance and provides insights into the structure-activity relationship for efficient biomass conversion. The findings suggest that the CdPS₃/CdS heterostructure is a promising catalyst for hydrogenation reactions, offering a sustainable alternative to traditional thermocatalytic methods.