Applications of nanoscale zero-valent iron (nZVI) in wastewater treatment demand fast and complete separation of nZVI for its reuse and to ensure high-quality effluent. Gravity settling is a promising candidate for nZVI separation due to its low capital and operational cost. Herein, we report polyacrylamide-enhanced separation of nZVI under quiescent and dynamic conditions. A considerable fraction (20-60 mg/L) of bare nZVI remained in supernatant as stable colloids, even with extended settling time of 3 h and very low overflow rate (0.1 m(3)/m(2) h). The addition of low dose PAM (<= 10 mg/g-nZVI) increased the settling efficiency of nZVI by nearly 5 times and improved the effluent quality as well. The colloidal iron in the supernatant was reduced to less than 5 mg/L; the mean hydrodynamic size of nZVI increased by nearly 60 times, from 7.6 mu m to 474 mu m, as measured by optical microscope and particle size analyzer. Low dosage (<= 10 mg-PAM/g-nZVI) of PAM reduced the surface charge (zeta potential) of nZVI while overdosing PAM (>= 50 mg-PAM/g-nZVI) may recharge and re-stabilize the iron nanopartides. No inhibition effect of PAM on nZVI reactivity was observed, likely due to its low surface coverage. The study demonstrates a reliable and cost-effective solution for nZVI separation and also proves that nZVI is fully compatible with conventional wastewater treatment processes. (C) 2014 Elsevier B.V. All rights reserved.