This study first demonstrated the possibility of the production of catalyst supports in the form of granules and tablets composed of nanoparticles of Fe atom cluster-doped CNTs using mini-mold forming and spark plasma sintering (SPS) techniques respectively. The pilot samples of the novel catalyst system containing 3% NiO active phase, synthesized on the granulated Fe cluster-doped CNTs carrier, were tested to determine their catalytic activity and coking resistance in the DRM reaction, in a wide range of temperatures up to 900oC. The developed novel catalyst systems’ samples were characterized before and after the catalyst reaction using SEM, EDX, XRD, and AES methods. It is shown that the temperature dependence of the catalytic activity of the 3% NiO catalyst, supported on the granulated Fe cluster-doped CNTs carrier, revealed two characteristic temperature ranges with different rates of efficiency. Particularly, at high reaction temperatures, starting from 700oC, the conversion rates of methane and carbon dioxide (42.4% and 45.6% respectively) have more than doubled at 850oC. Starting from 850oC to 900oC the latter tends to exceed the carbon dioxide conversion rate, and at 900oC it amounts to 95%.