2,5-diformylfuran (DFF) is a significant biomass derivative that is employed in a variety of industries. One approach to synthesizing it is through the oxidation of 5-hydroxymethylfurfural (HMF). The challenges in DFF production arise from the need for extreme conditions, issues with overoxidation, and the limitations of noble materials used in neutral or acidic environments. By using a mildly alkaline electrolyte, DFF can be produced electrochemically alongside hydrogen gas generation, eliminating extreme conditions and allowing for the study of a wide range of transition metals. Moreover, the performance of bimetallic electrocatalysts has been studied, and it has been found to be more active in many kinds of processes, particularly Layered Double Hydroxides (LDH). Electrodeposition, once widely chosen among various LDH production methods, is preferred for producing controlled and uniform thin layers. This work examines the electrocatalytic properties of NiCo-LDH and NiFe-LDH in the production of DFF. Cobalt, which exhibits strong adsorption, will be compared to iron, which has a weak adsorption characteristic toward HMF. This study demonstrates that NiCo-LDH gives 1.49 V vs. RHE onset potential, 600 mV lower compared to NiFe-LDH (1.55 V vs. RHE) for HMF oxidation reaction. NiCo-LDH also converts twice the amount of HMF compared to NiFe-LDH for the same amount of charge passed at 0.25 mA/cm−2 in 0.1 M Na2B4O7. However, strong adsorption promotes reactant activation and reduces the energy barrier while reducing DFF selectivity in NiCo-LDH (23.4%) due to overoxidation, compared to NiFe-LDH (31.6%). In order to achieve optimal electrocatalyst performance, a careful balance of adsorption strength and reaction pathway management is required. Proper optimization of these parameters is essential to improve efficiency and selectivity in the electrocatalytic process. © 2025 by the authors.