Green iron nanoparticles (G-nZVi) were synthesized in situ by adding grape-seed extracts and fe 2+ solution simultaneously. the performances for the removal of cr(Vi) were compared in a homogeneous system by original G-nZVi (in suspension) with in a heterogeneous system by treated G-nZVi. the characterization of teM, SeM, XRD, ftiR and XpS show that G-nZVi is the formation of fe°-iron oxide core-shell nanoparticles with organic matters in the extracts as capping/stabilizing agents. the same excellent performances on the removal of cr(Vi) were observed in the both systems and the adsorption capacity was from 78.3 to 166.7 mg (Cr)•g −1 (fe) with the increase of initial fe 2+ concentrations. the pseudo second-order model described the adsorption process excellently and both pseudo first-order and pseudo second-order models fit the reduction process well. It illustrated that the reaction included prompt adsorption and simultaneous redox process. Moreover, the results of thermodynamics study (ΔG° < 0, ΔH° > 0, ΔS° > 0) revealed that the adsorption was a spontaneous and endothermic process. it is obvious that the systhesis of original G-nZVi in the homogeneous system is more simple, rapid, cost-effective and suitable for in situ uses. it holds a great potential for remediation of soil and water. Chromium is one of the most common heavy metals because of its chemical stability and low biodegradability 1-3. Hexavalent chromium (Cr(VI)) is 100-fold times more toxic than trivalent chromium (Cr(III)) and highly soluble in water 4. Hence, Cr(VI) can get into aquatic ecosystems such as underground water and contaminate drinking water 5,6. Various chemical and physical treatments are employed for the Cr(VI) removal from the aqueous solution, such as membrane separation 7 , coagulation and flocculation 8 , adsorption and biosorption treatments 9-11 , Among the treatments, adsorption technique is advantageous due to its effectiveness, easiness in operating and less generation of chemical sludge. In the current trend, nanotechnology has been widely preferred because of the huge specific surface area 12. Nano-scale zero-valent iron (nZVI) plays a crucial role for environmental remediation due to its strong reducing power and its ability to adsorb many important contaminants such as heavy metals 13. In fact, the most suitable method of Cr(VI) removal should include the reduction of Cr(VI) to Cr(III), since Cr(III) is significantly less toxic, much lower aqueous solubility and mobility than Cr(VI). Hence, nZVI based techniques have been widely employed in the removal of Cr(VI) 14,15. However, nZVI particles tend to aggregate rapidly and thereby reduce the specific surface area and diminish particles reactivity. Various stabilization techniques have been applied to improve nZVI dispersibility, such as protective coatings 3,16 and solid supports 9,10,17. In recent years, green synthesis of nZVI has been received growing attention and developed as a promising alternative for chemical and physical methods, due to its advantages of a sim...