This study investigates the electrocatalytic hydrogenation of 5-hydroxymethylfurfural (HMF) to 2,5-bis(hydroxymethyl)furan (BHMF) using a two-dimensional (2D) layered CdPS₃ nanosheet electrocatalyst. The in-situ surface reconstruction of CdPS₃ nanosheets, triggered by electrolyte, facilitates efficient BHMF production under ambient conditions. Raman spectroscopy and post-mortem catalyst characterizations reveal the formation of a surface-bounded CdS layer on CdPS₃, forming a CdPS₃/CdS heterostructure. This electrocatalyst demonstrates high catalytic activity, achieving a Faradaic efficiency (FE) of 91.3 ± 2.3% and a yield of 4.96 ± 0.16 mg/h for BHMF at −0.7 V versus reversible hydrogen electrode (V_BHE). Density functional theory (DFT) calculations show that the CdS layer optimizes the adsorption of HMF* and H* intermediates, facilitating the HMF hydrogenation process. When coupled with MnCo₂O₄.₅ as the anode, the system enables simultaneous BHMF and formate synthesis from HMF and glycerol substrates with high efficiency. The study highlights the importance of in-situ surface reconstruction in enhancing the catalytic performance of 2D nanosheet electrocatalysts for efficient biomass hydrogenation.This study investigates the electrocatalytic hydrogenation of 5-hydroxymethylfurfural (HMF) to 2,5-bis(hydroxymethyl)furan (BHMF) using a two-dimensional (2D) layered CdPS₃ nanosheet electrocatalyst. The in-situ surface reconstruction of CdPS₃ nanosheets, triggered by electrolyte, facilitates efficient BHMF production under ambient conditions. Raman spectroscopy and post-mortem catalyst characterizations reveal the formation of a surface-bounded CdS layer on CdPS₃, forming a CdPS₃/CdS heterostructure. This electrocatalyst demonstrates high catalytic activity, achieving a Faradaic efficiency (FE) of 91.3 ± 2.3% and a yield of 4.96 ± 0.16 mg/h for BHMF at −0.7 V versus reversible hydrogen electrode (V_BHE). Density functional theory (DFT) calculations show that the CdS layer optimizes the adsorption of HMF* and H* intermediates, facilitating the HMF hydrogenation process. When coupled with MnCo₂O₄.₅ as the anode, the system enables simultaneous BHMF and formate synthesis from HMF and glycerol substrates with high efficiency. The study highlights the importance of in-situ surface reconstruction in enhancing the catalytic performance of 2D nanosheet electrocatalysts for efficient biomass hydrogenation.