A continuous electrocatalytic reactor offers a promising method for producing fuels and value-added chemicals via electrocatalytic hydrogenation of biomass-derived compounds. However, such processes require a better understanding of the impact of different types of active electrodes and reaction conditions on electrocatalytic biomass conversion and product selectivity. In this work, Ni1−xPdx (x = 0.25, 0.20, and 0.15) alloyed nanostructures were synthesized as heterogeneous catalysts for the electrocatalytic conversion of furfural. Various analytical tools, including XRD, SEM, EDS, and TEM, were used to characterize the Ni1−xPdx catalysts. The alloyed catalysts, with varying Ni to Pd ratios, showed a superior electrocatalytic activity of over 65% for furfural conversion after 4.5 h of reaction. In addition, various experimental parameters on the furfural conversion reactions, including electrolyte pH, furfural (FF) concentration, reaction time, and applied potential, were investigated to tune the hydrogenated products. The results indicated that the production of 2-methylfuran as a primary product (S = 29.78% after 1 h), using Ni0.85Pd0.15 electrocatalyst, was attributed to the incorporation of palladium and thus the promotion of water-assisted proton transfer processes. Results obtained from this study provide evidence that alloying a common catalyst, such as Ni with small amounts of Pd metal, can significantly enhance its electrocatalytic activity and selectivity.