This study demonstrates that in-situ surface reconstruction of a two-dimensional layered CdPS<sub>3</sub> nanosheet electrocatalyst, triggered by electrolyte, facilitates efficient 5-hydroxymethylfurfural (HMF) hydrogenation to 2,5-bis(hydroxymethyl)furan (BHMF) under ambient conditions. In-situ Raman spectroscopy and catalyst characterizations reveal the formation of a surface-bounded CdS layer, creating a CdPS<sub>3</sub>/CdS heterostructure. This electrocatalyst achieves a Faradaic efficiency for BHMF of 91.3 ± 2.3% and a yield of 4.96 ± 0.16 mg/h at -0.7 V versus reversible hydrogen electrode. DFT calculations show the CdPS<sub>3</sub>/CdS interface optimizes HMF* and H* adsorption, improving HMF hydrogenation. Coupling the CdPS<sub>3</sub>/CdS cathode with a MnCo<sub>2</sub>O<sub>4</sub> anode enables simultaneous BHMF and formate synthesis from HMF and glycerol.