Phytoremediation is considered an effective strategy for remediation of heavy-metal-contaminated soil in mining areas. However, single-species plants cannot reach the highest potential for uptake of heavy metals due to inhibition of their growth by high concentrations of heavy metals in the soil. Therefore, this study has explored the effects of illite application and two plant species’ co-cropping on soil quality, plant growth, and heavy metal transformation in a soil–plant system. The results reveal that the addition of 1% (mass fraction) of illite significantly enhances soil pH. The co-cropping of Ilex cornuta and Epipremnum aureum is beneficial for improving the organic matter content of the soil. The contents of EDTA-extractable Pb, Zn, and Cu were significantly reduced by 29.8–32.5%, 1.85–5.72%, and 30.0–32.9%, respectively, compared to the control. The co-cropping of Ilex cornuta and Epipremnum aureum promoted enrichment effects of Epipremnum aureum on Pb and Ilex cornuta on Cd (p < 0.05). The co-cropping pattern lowered the biomass of Ilex cornuta and Epipremnum aureum; however, co-cropping of Ilex cornuta and Epipremnum aureum promoted the elimination of Pb, Zn, Cu, and Cd from the soil at 13.0–75.8%, 11.1–38.2%, 8.39–88.4%, and 27.8–72.5%, respectively. It is concluded that illite application combined with co-cropping of Ilex cornuta and Epipremnum aureum is highly effective for the elimination of Pb, Zn, Cu, and Cd from contaminated soil. This study provides a theoretical basis and pathway for the restoration of heavy-metal-contaminated soil in mining with the application of bentonite combined with phytoremediation.