Ni‐promoted electrocatalytic biomass reforming has shown promising prospect in enabling high value‐added product synthesis. Here, we developed a novel hybrid catalyst with Ni nanosheet forests anchored on carbon paper. The hybrid catalyst exhibits high efficiency in electrooxidation of HMF to FDCA coupling with H2 production in high purity. The Ni nanosheets have small crystal grain sizes with abundant edges, which is able to deliver an efficient HMF oxidation to FDCA (selectivity >99 %) at low potential of 1.36 VRHE with high stability. The post‐reaction structure analysis reveals the Ni nanosheets would transfer electrons to carbon and readily turn into NiOx and Ni(OH)x during the reaction. DFT results suggest high valence Ni species would facilitate the chemical adsorption (activation) of HMF revealing the reaction pathway. This work emphasizes the importance of the precise control of Ni activity via atomic structure engineering. Highly efficient and stable electro‐reforming of HMF into FDCA on a Ni nanosheet/carbon paper electrode is achieved at a potential of 1.36 VRHE with 99.7 % conversion. A precursor‐limiting electrodeposition method creates a unique Ni nanosheet forest structure with vastly different physical appearance and catalytic activity comparing with conventional Ni catalysts.