To modify the surface characters, carbon whiskers were oxidized with carbon dioxide. Adsorption isotherms were determined by using three kinds of adsorbates: nitrogen, n-butane, and trichloroethylene (TCE). Granular activated carbon was used as the standards of adsorbents. The surface chemical structures were analysed by using NaHCO3, Na2CO3, and NaOH. After CO2 oxidation treatment of carbon whiskers, micropore structures of pore size distribution, having a sharp peak at a radius of 4 × 10−10 m were developed, but acidities of acidifie functional group were not increased. The oxidized carbon whiskers were better than the granular activated carbon for adsorption of TCE from aqueous solution.