A catalyst production method that enables the independent tailoring of the structural properties of the catalyst, such as pore size, metal particle size, metal loading or surface area, allows to increase the efficiency of a catalytic process. Such tailoring can help to make the valorization of CO2 into synthetic fuels on Ni catalysts competitive to conventional fossil fuel production. In this work, a new spray-drying method was used to produce Ni catalysts supported on SiO2 and Al2O3 nanoparticles with tunable properties. The influence of the primary particle size of the support, different metal loadings, and heat treatments were applied to investigate the potential to tailor the properties of catalysts. The catalysts were examined with physical and chemical characterization methods, including X-ray diffraction, temperature-programmed reduction, and chemisorption. A temperature-scanning technique was applied to screen the catalysts for CO2 methanation. With the spray-drying method presented here, well-organized porous spherical nanoparticles of highly dispersed NiO nanoparticles supported on silica with tunable properties were produced and characterized. Moreover, the pore size, metal particle size, and metal loading can be controlled independently, which allows to produce catalyst particles with the desired properties. Ni/SiO2 catalysts with surface areas of up to 40 m2 g−1 with Ni crystals in the range of 4 nm were produced, which exhibited a high activity for the CO2 methanation.