The effect of nickel content on NiO-MgO-ZrO2 catalysts was investigated. They were characterized by XRD, in-situ XRD, TPR and BET and tested in POM and DRM coupled reactions (1.5CH4:1CO 2:0.25O2), to produce syngas (H2/CO), at 750°C for 7 h. Among these catalysts the NiO-MgO-ZrO2 catalyst with 20 wt.% nickel content showed the best activity and selectivity in the catalytic processes. The MgO-ZrO2 (MZ) solid solution and the interactions between Ni and MZ increased the rate of conversion of reactants (CH4 and CO2) into syngas on the catalysts. Although the Ni°active sites are required for high activity and selectivity, high nickel content favored the formation of large Ni°particles during the reforming reaction, thus lowering the catalytic performance. The combination of DRM and POM exhibited high conversion rates and selectivity on the NiMZ catalyst with 20 wt.% Ni and 20 mol% MgO, demonstrating that this coupled reaction can be performed efficiently and that problems arising from hot spots on the catalyst, due to POM, can be solved. © 2012 Elsevier B.V.