Herein, we report a novel binder-free polyaniline coated 3D crumpled CoSe2 nanoparticles on Ni foam (CoSe2/PANI/NF) electrode developed by a simple co-electrodeposition process for methanol oxidation application. The as-electrodeposited 3D CoSe2 with PANI films on Ni foam morphology was confirmed through in-depth material characterizations. As a non-noble electro-catalyst for methanol oxidation, the CoSe2/PANI/NF electrode showed high current density of 139 mA cm−2, low onset potential and no decay in the current response over 3000 s at 0.5 V. The high electrochemical performance of the electrode is due to the synergistic effect between PANI and CoSe2 nanostructures, high electrical conductivity, and hydrophilic functional groups of PANI contributing to the low internal resistance and effective diffusion of ions. These results demonstrate that the CoSe2/PANI/NF with its unique 3D morphology has great potential in energy storage and catalytic applications. © 2021 Elsevier B.V.