A simple method for surface ion-imprinting is described in which poly(glycidyl methacrylate) is grafted onto PP fibers to act as a binder to a Cu2+ ion-imprinted polymer layer. Mechanical and thermal analysis shows excellent tensile and thermal properties of the ion-imprinted fibers. Competitive adsorption of Cu2+ and other ions such as Zn2+, Ni2+, Cd2+, Mn2+, and Mg2+ on the fibes is examined and a highly selective adsorption of Cu2+ is observed. The selectivity coefficient for Cu2+ with respect to Cd2+ can be as high as 20.2. Dynamic adsorption results indicate that the fibers are able to thoroughly remove Cu2+ from a solution. Regeneration performance tests show that the fibers maintain almost the same adsorption capacity for copper ions after 10 adsorption/desorption cycles.