Soil contamination by Cr(VI) has attracted widespread attention globally in recent years, but it remains a significant challenge in developing an environmentally friendly and eco-sustainable technique for the disposal of Cr(VI)-contaminated soil. Herein, a sustainable cyclic soil washing system for Cr(VI)-polluted soil remediation and the recovery of washing agents using biochar supported nanoscale zero-valent iron (nZVI-BC) was established. Citric acid (CA) was initially screened to desorb Cr(VI) from contaminated soil, mobilizing Cr from the highly bioaccessible fractions. The nZVI-BC exhibited superior properties for Cr(VI) and Cr(total) removal from spent effluent, allowing effective recovery of the washing agents. The elimination mechanism of Cr(total) by nZVI-BC involved the coordinated actions of electrostatic adsorption, reduction, and co-precipitation. The contributions to Cr(VI) reduction by Fe, surface-bound Fe(II), and soluble Fe(II) were 0.6 %, 39.8 %, and 59.6 %, respectively. Meanwhile, CA favored the activity of surface-bound Fe(II) and Fe in nZVI-BC, enhancing the production of soluble Fe(II) to strengthen Cr(VI) removal. Finally, the recovered washing agent was proven to be reused three times. This study showcases that the combined soil washing using biodegradable chelant CA and effluent treatment by nZVI-BC could be a sustainable and promising strategy for Cr(VI)-contaminated soil remediation.