The remediation of Cr(VI) from simulated water streams is investigated using Fe-Ni bimetallic nanoparticles (Fe-Ni NPs) and their nanocomposites prepared with montmorillonite (MMT) clay. These nanocomposites are characterized using X-ray diffraction (XRD), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS) and Brunauer-Emmett-Teller (BET) surface area analyses. XRD analysis revealed proper dispersion as well as intercalation of Fe-Ni NPs in the clay matrix. TEM of nanocomposites showed the presence of spherical particles having a size of 20-40 nm. Batch experiments with a 25 mg L-1 Cr(VI) solution and 2 g L-1 Fe-Ni NPs exhibited complete reduction of Cr(VI) within 10 min that follows first order reaction kinetics. Amongst 25%, 50%, 75% in situ and loaded nanocomposites, 75% compositions possess better activity with enhanced reduction capacity below pH 4 due to generation of reactive H center dot species. XPS analysis of nanocomposites after Cr(VI) treatment suggested that reduction process occurs through Cr(111) formation followed by its subsequent reduction to Cr(0). Their potentiality towards reusage is established from the recycling experiments that revealed the order of efficiency as 75% in situ > Fe-Ni NPs > 75% loaded nanocomposites. (C) 2011 Elsevier B.V. All rights reserved.