Technetium-99 (Tc-99) is a major contaminant at nuclear power plants and several US Department of Energy sites. Its most common aqueous species, pertechnetate (TcO4-), is very mobile in the environment, and currently there are no effective technologies for its sequestration. In this work, a porous iron (pFe) material was investigated for TcO(4)(- )and perrhenate (ReO4-) sequestration from artificial groundwater. The pFe was significantly more effective than granular iron for both TcO4- and ReO4- sequestration under oxic conditions. The Tc removal capacity was 27.5 mg Tc/g pFe at pH (similar to)6.8, while the Re removal capacity was 23.9 mg Re/g pFe at pH (similar to)10.6. Tc K-edge XANES and EXAFS analyses indicated that the removed Tc species was 70-80% Tc(IV) that was likely incorporated into Fe corrosion products (i.e., Fe(OOH), Fe3O4) and 20-30% unreduced TcO4-. In contrast, the removed Re species was ReO4- only, without detectable Re(IV). In addition, the sequestered ReO4- was not extracted (< 3%) by 0.1 M Na2SO4 and 1 M KI solution, which indicated that ReO4- and by chemical analogy, unreduced TcO4-, was likely incorporated into Fe corrosion products. This inexpensive pFe material may be applied to the sequestration and stabilization of (TcO4-)-Tc-99 from contaminated environments and nuclear waste streams.