Electrocatalytic oxidation of furfural to furoic acid offers a sustainable route for biomass valorization, yet remains challenged by sluggish kinetics and limited stability. Herein, a hierarchical core–shell CoFe@NiFe-LDH/NF heterostructure was fabricated on nickel foam via a hydrothermal-electrodeposition method. Vertically aligned CoFe-LDH nanosheets induce directional growth of NiFe-LDH, and XPS confirms strong electronic interactions and interfacial charge rearrangement.