Fibrous adsorbents, such as activated carbon fibers (ACF) have acknowledged advantages of rapid adsorption rate and ease of modification compared with granular and powdered adsorbents. Based on the surface modification of lyocell-based ACF, we observed different surface characteristics of ACF samples with variation in the mixing ratio and impregnation time of H3PO4, NaCl, and KMnO4 solution. For an engineering application, we also explored the adsorption characteristics of thusproduced ACF samples onto volatile organic compounds (VOCs). Isothermal adsorption experiments were performed using toluene and benzene as adsorbates. Results indicate that both physical and chemical surface properties have an effect on the adsorption of volatile organic compounds (VOCs).