Nickel (Ni) impregnated activated carbon fibers (ACFs) were used as a substrate to grow carbon nanofibers (CNFs) for the removal of persistent gaseous organic pollutants. A surfactant (cetyl trimethylammonium bromide) was used in the impregnating solution of nickel nitrate hexahydrate, which helps to create much smaller and denser Ni particle (catalyst) distribution on ACF for CNF-growth. Temperature programmed reduction, atomic absorption spectroscopy, X-ray diffraction spectroscopy, and adsorption tests were used to characterize and compare the products. Scanning electron microscopy and H-2-chemisorption were used to investigate the surface morphology and the active metal sites, respectively, of the prepared adsorbent. The adsorption performance of ACF/CNF evaluated under flow conditions established that the adsorption of the gaseous pollutant was larger on the CNFs prepared using the surfactant than on the CNFs grown without using the surfactant.