Treatment of wastewater containing heavy metals requires considerations on simultaneous removal of different ions, system reliability and quick separation of reaction products. In this work, we demonstrate that nanoscale zero-valent iron (nZVI) is an ideal reagent for removing heavy metals from wastewater. Batch experiments show that nZVI is able to perform simultaneous removal of different heavy metals and arsenic; reactive nZVI in uniform dispersion brings rapid changes in solution E-h, enabling a facile way for reaction regulation. Microscope characterizations and settling experiments suggest that nZVI serves as solid seeds that facilitate products separation. A treatment process consisting of E-h-controlled nZVI reaction, gravitational separation and nZVI recirculation is then demonstrated. Long-term (>12 months) operation shows that the process achieves >99.5% removal of As, Cu and a number of other toxic elements. The E-h-controlled reaction system sustains a highly-reducing condition in reactor and reduces nZVI dosage. The process produces effluent of stable quality that meets local discharge guidelines. The gravitational separator shows high efficacy of nZVI recovery and the recirculation improves nZVI material efficiency, resulting in extraordinarily high removal capacities ((245 mg As + 226 mg-Cu)/g-nZVI). The work provides proof that nanomaterials can offer truly green and cost-effective solutions for wastewater treatment. (C) 2016 Elsevier B.V. All rights reserved.