this study fabricated novel heteroaggregates of montmorillonite (Mt) microparticles with nanoscale zero-valent iron (nZVi) (Mt-nZVi) and examined the removal of cr(Vi) by the Mt-nZVi through batch experiments. Spherical nZVi particles were synthesized by the liquid phase reduction method, which were then attached on the flat Mt surfaces in monolayer. The fabricated Mt-nZVI had similar removal efficiency for Cr(VI) compared to the monodispersed nZVI particles, but was much greater than that of nZVI aggregates. The removal efficiency of Mt-nZVI increased with decreasing its dosage and increasing initial Cr(VI) concentration, whereas had insignificant change with solution pH. the removal of cr(Vi) by Mt-nZVi was well described by the pseudo second-order kinetics and the Langmuir equilibrium model. the removal was spontaneous and exothermic, which was mainly due to chemsorption rather than intra-particle diffusion according to calculation of change in free energy and enthalpy and Weber-Morris model simulations. X-ray diffraction and X-ray photoelectron spectroscopy analysis revealed that the adsorption was likely due to reduction of cr(Vi) to cr(iii) by Fe(0) and co-precipitation in the form of oxide-hydroxide of Fe(III) and Cr(III). The fabricated Mt-nZVI showed the promise for in-situ soil remediation due to both high removal efficiency and great mobility in porous media. Nanoscale zero-valent iron (nZVI) has been shown to be very effective for treatment of various inorganic and organic pollutants in water in the past two decades 1,2 , due to its unique properties such as large specific surface area and high surface activity. However, the nZVI particles are readily to aggregate in water during the preparation and application because of attractive van der Waals force, high surface energy, and magnetic attractive force 3. The aggregation reduces specific surface areas of the nZVI, which can significantly decrease its reactivity and efficiency for treatment of contaminants 4. The aggregation also reduces the mobility of the nZVI in subsurface environments such as soil by sedimentation and straining at narrow pores 5 , and hence greatly limits its application for in-situ soil remediation. Various techniques have been developed to prevent nZVI aggregation and enhance its dispersion 6,7. For example, functional groups have been added on surfaces of nZVI via chemical modification (covalent or noncovalent functionalization) 8. Adding functional groups increases surface charge, and consequently enhances electrostatic repulsion between nZVI particles in electrolyte solutions and their dispersion. In addition, polymers and surfactants have been used to stabilize the nZVI particles by inducing the steric repulsion between them 9. However, it should be noted that adding functional groups or coating of these additives on nZVI particles masks the particle surfaces, which may decrease the efficiency of nZVI for contaminant treatment compared to bare monodispersed nZVI particles 10,11 .