In order to study the desulfurization performance of activated carbon fibers (ACF) with N-surface modified, surface modified ACF with nitrogen-containing group were prepared by heat-treatment of ACF with urea. Samples were characterized by SEM, XPS, and TG, and the desulfurization activities were tested. The results showed that the sample prepared under the heat treatment temperature of 750 ℃ and the urea concentration of 2.4 mol/L has the best desulfurization activity. The number of nitrogen surface functional groups of ACF were increased by the impregnation of urea and treatment under high temperature, especially pyridine nitrogen increased nearly five times.The ACF modified by nitrogen-functional groups has good desulfurization activity.