<p>The electrooxidation of ethylene glycol (EG) to formate converts low-cost raw materials into high-value chemicals, promoting green chemistry, reducing fossil fuel dependence and supporting sustainable production. Currently, there are still several challenges, including inadequate catalyst stability, room for improvement in faradaic efficiency, and difficulties in controlling oxidation. Herein, needle-like Co₃Fe₁-LDH/NF was employed for highly selective ethylene glycol oxidation reaction (EGOR) to formate. The Co₃Fe₁-LDH/NF with abundant active sites and fast transfer kinetics, possessed an outstanding formate selectivity of 93.09% and a record faradaic efficiency of 98.48% at a current density of 100&#xa0;mA&#xa0;cm⁻². The Co₃Fe₁-LDH underwent a potential-driven surface reconstruction into Co-/Fe-OOH active species in EGOR, accompanied by a morphological transition to a sheet-like nanoarchitecture. Meanwhile, the anodic oxidation of EG promoted the hydrogen production by 1.17 times. Overall, the Co₃Fe₁-LDH/NF proved to be a simple electrochemical catalyst to achieve highly selective oxidation of ethylene glycol to formate.</p> Graphical abstract <p></p>