The one-step method of carbon nanotubes filled with continuous cobalt nanowires (CoF-CNT) synthesis is presented. Co/ZSM-5 (8 wt% Co) was used as catalyst for CoF-CNT production by methane decomposition at the temperature of 400°C and 800°C at atmospheric pressure in a conventional gas-flow system. The average diameter of the CoF-CNT is about 25 and 40 nm for products obtained at 400°C and at 800°C, respectively. The average size of coherently scattering domains along the normal to graphite layers L c , the interlayer spacing d 002 , the graphitization degree of carbon, and the relative intensities of the G and D bands in Raman spectroscopy were determined to characterize the quality of carbon. It was proved that cobalt-filled carbon nanotubes can be produced by a simple method. The results of XRD, FE-SEM, and TEM show that CoF-CNT can be obtained even at 400°C by catalytic decomposition of methane. On the basis of XRD, TEM, Raman spectroscopy was found that at a temperature of 800°C, a better quality of carbon was produced.