Permeable-reactive redox walls, placed below the ground surface in the path of flowing groundwater, provide an alternative remediation approach for removing electroactive chemicals from contaminated groundwater. Four types of Fe-bearing solids, siderite [FeCO3], pyrite [FeS2], coarse-grained elemental iron [Fe-0], and fine-grained Fe-0, were assessed for their ability to remove dissolved Cr(VI) from solution at flow rates typical of those encountered at sites of remediation. Batch studies show that the rate of Cr(VI) removal by fine-grained Fe-0 is greater than that for pyrite and coarse-grained Fe-0. Results from column studies suggest that partial removal of Cr(VI)) by pyrite and coarse-grained Fe-0 and quantitative removal of Cr(VI) by fine-grained Fe-0 occur at rapid groundwater flow velocities. The removal mechanism for Cr(VI) by fine-grained Fea and coarse-grained Fe-0 is through the reduction of Cr(Vl) to Cr(III), coupled with the oxidation of Fe-0 to Fe(II) and Fe(III), and the subsequent precipitation of a sparingly soluble Fe(III)-Cr(III) (oxy)hydroxide phase. Mineralogical analysis of the reactive material used in the batch tests indicates that Cr is associated with goethite(alpha-FeOOH). These results suggest th at Cr(lll) is removed either th ro ugh the formation of a solid solution or by adsorption of Cr(III) onto the goethite surface. The effective removal of Cr(VI) by Fe-0 under dynamic flow conditions suggests porous-reactive walls containing Fe-0 may be a viable alternative for treating groundwater contaminated by Cr(VI).