Carbon nanomaterials were prepared from methane by catalytic decomposition over a nickel-supported ZSM-5 catalyst. The mole ratio of SiO2 to Al2O3 in ZSM-5 was 200-400. The nickel content was varied from 17 to 23 wt% Ni. In order to find the greatest yield and the highest quality of carbon nanomaterials the simplex design method for planning the experiments was applied. Different parameters such as: temperature, methane flow, nitrogen flow and nickel content in the catalyst were evaluated. The carbon nanomaterials were analyzed by the Raman spectroscopy, scanning and transmission electron microscopy, and total organic carbon analyzer.