Electrochemical oxidation of biomass-derived platform molecules can enable the production of value-added oxygenated commodity chemicals under mild conditions in a distributed fashion using renewable electricity; however, very few efficient, robust, and inexpensive electrocatalysts are available for such electrochemical oxidation. Here we demonstrate that earth-abundant NiFe layered double hydroxide (LDH) nanosheets grown on carbon fiber paper can efficiently catalyze the oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) at the anode of an electrochemical cell. A near-quantitative yield of FDCA and 99.4% Faradaic efficiency of HMF conversion under ambient conditions can be achieved in the electrochemical process. HMF has a higher rate of oxidation than water and can act as an alternative anodic reaction for alkaline H2 evolution in water-splitting cells. As the first report on using bimetallic metal hydroxide/oxide catalysts for electrochemical oxidation of HMF, this work opens up opportunities in electrochemical devices to simultaneously produce building-block chemicals from biomass-derived molecules and clean H2 fuels under ambient conditions with earth-abundant materials.