The methanation of CO2 is of great interest in power-to-gas systems and contributes to the mitigation of climate change through carbon dioxide capture and the subsequent production of high-added-value products. This study investigated CO2 methanation with three Ni catalysts supported on Al2O3 and ZrO2, which were simulated using a mathematical model of a packed bed reactor designed based on their chemical kinetics reported in the literature. The simulated reactive system was fed with syngas obtained from residual coffee pulp obtained after a solvent phytochemical extraction process under several gasification conditions. The results reflect a high degree of influence of the catalyst support, preparation method, and syngas composition on CO2 and H2 conversions and CH4 selectivity. For all the syngas compositions, the Ni/ZrO2 catalysts showed the best values for CO2 conversion and H2 conversion for the Ni/Al2O3 catalyst except in gasification at 700 °C and using the Ni/ZrO2p catalyst.