In this paper, a novel approach to the synthesis of the carbon nanotubes (CNTs) in reactors operating at atmospheric pressure is presented. Based on the literature and our own research results, the most effective methods of CNT synthesis are investigated. Then, careful selection of reagents for the synthesis process is shown. Thanks to the performed calculations, an optimum composition of gases and the temperature for successful CNT synthesis in the CVD (chemical vapor deposition) process can be chosen. The results, having practical significance, may lead to an improvement of nanomaterials synthesis technology. The study can be used to produce CNTs for electrical and electronic equipment (i.e., supercapacitors or cooling radiators). There is also a possibility of using them in medicine for cancer diagnostics and therapy.