The challenge in the electrochemical reduction of levulinic acid (LA) lies in designing highly selective, energy-efficient, and non-precious-metal electrocatalysts that minimize the competitive hydrogen evolution reaction during LA conversion. Herein, we reported a facile pulsed electrodeposition strategy to fabricate bimetallic electrocatalysts with different combinations of lead (Pb), indium (In), tin, and cadmium supported by free-standing carbon felts (CFs). The as-prepared bimetallic self-supporting electrodes were examined for the electrochemical hydrogenation (ECH) of LA. The resulting InPb/CF electrocatalysts showed superior performance among the bimetallic catalysts. In addition, it was demonstrated that the catalytic performance of bimetallic samples was better than that of the corresponding monometallic samples. Notably, the In72.4Pb27.6/CF exhibited the best performance for ECH of LA, leading to 86.1 % of LA conversion, 99.7 % of selectivity towards valeric acid and 60.8 % of Faradaic efficiency at −1.5 V vs RHE. The excellent performance is mainly attributed to the modification of the electronic structures by the ligand and strain effects. Meanwhile, the relatively high electrochemically active surface area and the low charge transfer resistance are also conducive to improving the catalytic performance.