Novel versatile nanomaterials may facilitate strategies for simultaneous soil remediation and agricultural production, but a thorough and mechanistic assessment of efficacy and safety is needed. We have established a new soil remediation strategy using nanoscale zero-valent iron (nZVI) coupled with safe rice production in paddy soil contaminated with pentachlorophenol (PCP). In comparison with rice cultivation in contaminated soil with 100 mg PCP per kg soil but without nZVI, the addition of 100 mg nZVI per kg soil increased grain yield by 47.1-55.0%, decreased grain PCP content by 83.6-86.2% and increased the soil PCP removal rate from 49.9 to 83.9-89.0%. The specific role of nZVI-derived root iron plaque formation in the safe production of rice has been elucidated, and the synergistic effect of nZVI treatment and rice cultivation identified in the nZVI-facilitated rhizosphere microbial degradation of PCP. This work opens a new strategy for the application of nanomaterials in soil remediation that could simultaneously enable safe crop production in contaminated lands. The application of nanoscale zero-valent iron simultaneously increased rice production and rhizoremediation of pentachlorophenol-contaminated soil.