Nanoscale zero-valent iron (nZVI) has been broadly applied in the remediation of heavy metals pollution. In this research, the toxicity characteristic leaching procedure (TCLP), the in vitro gastrointestinal (IVG) method, and the diffusive gradients in thin-films (DGT) technique were used to evaluate the effects of heavy metals in soil with remediation by nZVI. The results indicate that, compared with the dose of 0.5 g·L⁻¹, the nZVI in the dose of 1.0 g·L⁻¹ can remove the heavy metals in the soil. The leaching toxicities of the heavy metals (Cr, Cu, Zn, Pb) showed apparent decreases after the remediation by nZVI. In the gastric phase, the highest bioaccessibility values of the Cr, Cu, Zn, Pb were decreased by 27.2, 31.7, 11.7, and 20.1%, respectively. Moreover, in the gastric phase, the highest bioaccessibility values of the Cr, Cu, Zn, Pb were decreased by 5.5, 1.29, 8.0, and 7.3%, respectively. The availabilities of the heavy metals were also reduced. The above results show that the nZVI effectively reduced the heavy metal pollution in the soil.