Selective ion exchange is one of the preferred treatment technologies for removing low levels of perchlorate (ClO4-) from contaminated water because of its high efficiency and minimal impact on water quality through the addition or removal of chemicals and nutrients. However, the exceptionally high affinity of ClO4- for type I anion-exchange resins makes regeneration with conventional NaCl brine extremely difficult and costly for practical applications. The present study entails the development of a novel regeneration methodology applicable to highly selective anion-exchange resins. Tetrachloroferrate (FeCl4-) anions, formed in a solution of ferric chloride and hydrochloric acid (e.g., 1 M FeCl3 and 4 M HCl), were found to effectively displace Cl04- anions that were sorbed on the resin. A mass-balance analysis indicated that a nearly 100% recovery of ion-exchange sites was achieved by washing with as little as approximately 5 bed volumes of the regenerant solution in a column flow-through experiment There was no significant deterioration of the resin's performance with respect to ClO4- removal after repeated loading and regeneration cycles. Thus, the new methodology may offer a cost-effective means to regenerate ClO4- -loaded resins with improved regeneration efficiency, recovery, and waste minimization in comparison with conventional brine regeneration techniques.