The development of modern thermocatalytic technologies for processing oil and gas raw materials is one of the promising areas for the advancement of chemical production. New highly efficient catalytic systems with the required technical characteristics and long service life play an essential role in solving these issues. The paper focuses on obtaining propylene by selective propane dehydrogenation. In the course of the experiments, composite iron-containing catalysts were synthesized, in which the active component is iron oxide in combination with an inert carbon matrix. FAS activated carbon and carbon nanotubes were used as the matrix. As a result of the synthesis on the catalyst surface it was possible to obtain catalytic centers that transfer electrons by changing the degree of iron oxidation when converting the starting materials into the target reaction products. Findings of research show that the obtained ironcontaining catalysts significantly increase the efficiency of the process in comparison with the efficiency of thermal cracking of propane. Thus, the Fe3+/FAS catalyst showed a conversion rate of the initial reagent of 68 % and a propylene selectivity of about 42 %. Further transition to catalytic systems based on singlelayer and doublelayer carbon nanotubes modified with iron oxide (Fe3+/CNTI and Fe3+/CNTII) made it possible to obtain propane conversion up to 37-40 % with a decrease in propylene selectivity to 29-30 %. Studies of the service life of the synthesized catalytic systems and the possibility of their regeneration show that, with account for the regeneration, the activity of the catalysts and the main technical characteristics of the propane-to-propylene cracking process remain unchanged for 10 working cycles. © 2021 Bauman Press. All rights reserved.