Methane dry reforming (MDR) converts greenhouse gases into syngas. Exploring active catalysts to achieve stable MDR performance is still a great challenge because of the sintering and carbon deposition that occur at high temperatures. In this study, we rationally synthesized Ni−Cu alloy nanoparticles (approximately 5 nm) and utilized electrostatic adsorption for the MDR reaction. The miniscule alloy catalysts had low carbon deposition and trace sintering features, which contributed to a more active and stable MDR reaction than achievable with a pure Ni catalyst. The performance depended on the Cu/Ni ratio, and the highest performance was obtained at a Cu/Ni weight ratio of 0.5:4, followed by ratios of 0.2:4 and 1.5:4. This is because adding a proper quantity of Cu promoted the activation of CO 2 , which enhanced the transformation of CH x into syngas on Ni atoms, while excessive Cu addition formed individual Cu nanoparticles, which influenced Ni atoms on the surface and made the activation of CH 4 harder. This work not only fabricated miniscule alloy nanoparticles but also demonstrated the importance of the Ni/Cu ratio for enhancing the MDR performance.