Methanol steam reforming (MSR) is an ideal option of on-board hydrogen production for proton-exchange membrane fuel cell (PEMFC) vehicles. Conventional pellet catalysts are prone to physical breakage in frequent vibrations during vehicle movements, while current structural catalysts typically bear the disadvantages of complex synthesis procedures and poor bonding of the catalyst to the substrate. Here, we synthesized copper mesh catalysts via a modified chronopotentiometry method. Commercial copper meshes served as electrodes in an electrolyte composed of copper-free nitrate solution, with Cu species dissolved into the electrolyte at an oxidative potential and deposited at a reductive potential. In addition, Zn(NO 3 ) 2 and Al(NO 3 ) 3 were added into the electrolyte during electrochemical synthesis, with Zn 2+ functioning as an electron promoter and Al 3+ functioning as a structure promoter. The synthesized CuZnAl mesh catalyst exhibits a H 2 yield of 478.4 mmol/(g cat •h) at 250 °C with a WHSV MeOH of 12 h −1 in the MSR reaction, which surpasses that of commercial Cu/ZnO/Al 2 O 3 catalysts. The CuZnAl mesh shows strong robustness under harsh conditions including frequent oxidation and ultrasonic vibration, highlighting its application potential toward PEMFC vehicles.