The production of synthetic natural gas in the context of power-to-gas is a promising technology for the utilization of CO₂. Ni-based catalysts supported on carbon nanotubes (CNTs) were prepared through incipient wetness impregnation and characterized using N₂ adsorption, X-ray diffraction (XRD), transmission electron microscopy (TEM), thermogravimetric analysis (TGA), and temperature-programmed reduction (TPR). The catalysts were tested for CO₂ methanation in the 200–400 °C temperature range and at atmospheric pressure. The results demonstrated that the catalytic activity increased with the addition of the CNTs and Ni loading. The selectivity towards CH₄ was close to 100% for the Ni/ZrO₂/CNT catalysts. Reduction of the calcined catalyst at 500 °C using H₂ modified the surface chemistry of the catalyst, leading to an increase in the Ni particles. The CO₂ conversion was dependent on the Ni loading and the temperature reduction in the NiO species. The 10Ni/ZrO₂/CNT catalyst was highly stable in CO₂ methanation at 350 °C for 24 h. Thus, CNTs combined with Ni and ZrO₂ were considered promising for use as catalysts in CO₂ methanation at low temperatures.