Green nanoscale zero iron (nZVI) on an oak wood biochar support was prepared from tea polyphenol (TP-nZVI-OB), and applied to the removal of hexavalent chromium (Cr(VI)) from aqueous solution. The effects of experimental parameters on the Cr(VI) removal were evaluated by varying the Fe/C mass ratio, contact time, initial pH, and initial Cr(VI) concentration. The Cr(VI) removal performance of the TP-nZVI-OB was optimized at an Fe/C mass ratio of 2:1. The initial pH significantly affected the Cr(VI) removal, and 99.9% of the Cr(VI) was eliminated at pH 2.0. The kinetic data were well fitted to a pseudo-second order model, indicating that Cr(VI) removal was dominated by chemisorption. The successful TP-nZVI -OB synthesis and effective Cr(VI) removal mechanisms were confirmed by multiple techniques. The reaction between Cr(VI) and TP-nZVI-OB (2:1) involved multiple processes (sorption, reduction and co-precipitation), clarifying that TP-nZVI-OB is a potentially superior composite for Cr(VI) treatment of contaminated aqueous solution. (C) 2019 Elsevier Ltd. All rights reserved.