Production of value-added chemicals and fuels from biomass via electrochemical methods has been of emerging interest in light of the increasing environmental, economic, and political challenges. Paired electrolysis, with anodic oxidation and cathodic reduction reactions pairing in a single electrochemical cell, offers an effective way to produce desired products in both electrodes, thus achieving complete electron economy. In this work, an efficient 5-hydroxymethylfurfural (HMF) paired electrolysis system is developed over a self-supported ultrathin Co₃O₄ nanoarray electrocatalyst for simultaneous production of value-added 2,5-dihydroxymethylfuran (DHMF) and 2,5-furandicarboxylic acid (FDCA). The as-designed paired electrolysis cell achieves a high HMF conversion and DHMF/FDCA selectivity at both anode and cathode without external hydrogen and oxygen input. A near-quantitative yield (95.7%) of FDCA and 78.8% yield of DHMF can be achieved in the paired electrolysis system, with a total Faradaic efficiency of 127%. This work will open up new opportunities in designing efficient electrochemical devices to simultaneously produce building-block chemicals from biomass-derived molecules in both anode and cathode.