Electrooxidation of 5-hydroxymethylfural (HMF) into 2,5-furandicarboxylicacid (FDCA) has been regarded as a promising sustainable approach to achieve value-added chemicals. However, it is still impeded by the unsatisfactory performance of electrocatalysts. Here, Cu 2 P 7 -CoP heterostructure nanosheets were reported to enable powerful HMF electrooxidation. The Cu 2 P 7 -CoP heterostructure nanosheets were fabricated by microwave-assisted deep eutectic solvent (DES) approach, along with subsequent phosphiding. The Cu 2 P 7 -CoP heterostructure nanosheets enabled a superb 100 % HMF conversion at 1.43 V (vs. RHE) with 98.8 % FDCA yield and 98 % Faradaic efficiency (FE), demonstrating its promising application in HMF electrooxidation. X-ray photoelectron spectroscopy (XPS) analysis, open-circuit potential (OCP) approach and density functional theory (DFT) calculation uncovered that the electron transfer and redistribution between Cu 2 P 7 and CoP improved the adsorption capacity of HMF and modulated the catalytic performance. This study not only offered a powerful electrocatalyst for HMF electrooxidation, but also provided a conceptually new strategy for the heterostructure catalyst design.