In this paper, a chlorination method is proposed for simultaneous purification and functionalization of carbon nanotubes, thus increasing their ability to use. Carbon nanotubes were obtained by CVD method through ethylene decomposition on the nanocrystalline iron or cobalt or bimetallic iron-cobalt catalysts. The effects of temperature (50, 250, and 450°C) in the case of carbon nanotubes obtained on the Fe-Co catalyst and type of catalyst (Fe, Co, Fe/Co) on the effectiveness of the treatment and functionalization were tested. The phase composition of the samples was determined using the X-ray diffraction method. The quantitative analysis of metal impurity content was validated by means of the thermogravimetric analysis. Using X-ray Photoelectron Spectroscopy (XPS), Energy Dispersive Spectroscopy (EDS) analysis, and also Mohr titration method, the presence of chlorine species on the surface of chlorinated samples was confirmed.