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Three‐dimensional (3D) nanoporous CuAg (NPCuAg) alloy catalysts with various Cu/Ag ratios are prepared by electrochemical dealloying of metallic glassy (MG) precursors. All dealloyed samples exhibit homogenous nanoporous structure and element composition distribution. After systematically evaluating their electrocatalytic performance toward MOR, it was found that the catalytic activity of the NPCuAg catalysts is enhanced along with the increase of Cu/Ag ratio, which may be attributed to the more exposed active reaction sites derived from high surface area of nanoporous structure and the optimal synergistic effect. Thus, the NPCu1.75Ag alloy catalyst presents the best methanol electro‐oxidation properties, including a high current density of 397.2 mA cm−2 and good operation stability that retaining 84.5 % catalytic activity even after 7200 s. These results outperform most reported copper‐based MOR catalysts in alkaline methanol solution. Considering these advantages, the designed electrodes are expected to be promising catalysts for alkaline DMFCs applications. [ABSTRACT FROM AUTHOR]