Stimulated by the capacity of Zn to improve the adoption of CO2 and CH4, we doped a Ni-supported ZrO2 catalyst with Zn to enhance its performance and stability in the dry reforming of methane. We prepared a set of catalysts with different Ni:Zn:Zr proportions and conducted extensive ex situ and in situ characterizations to prove that a Ni–Zn alloy was formed at 750 °C under reductive conditions. Combining a tailored morphology of the alloy nanoparticles, strong metal–support (ZnO–ZrO2) interactions, and additional oxygen vacancies created by Zn inclusion resulted in an enhanced catalyst with 15% higher initial activity and higher stability for over 100 h on stream than Zn-free catalyst. Our experimental and modeling results demonstrated that the catalyst with adjusted Ni:Zn:Zr proportion improves the adsorption and reaction rates of CH4 and CO2 while extending its lifetime through enhanced coke precursor gasification compared to its Zn-free counterpart.