A novel composite of montmorillonite-supported carboxymethyl cellulose-stabilized nanoscale iron sulfide (CMC@MMT-FeS), prepared using the co-precipitation method, was applied to remediate hexavalent chromium (Cr(VI))-contaminated soil. Cr(VI)-removal capacity increased with increasing FeS-particle loading. We tested the efficacy of CMC@MMT-FeS at three concentrations of FeS: 0.2, 0.5, and 1 mmol/g, hereafter referred to as 0.2 CMC@MMT-FeS, 0.5 CMC@MMT-FeS, and 1.0 CMC@MMT-FeS, respectively. The soil Cr(VI) concentration decreased by 90.7% (from an initial concentration of 424.6 mg/kg to 39.4 mg/kg) after 30 days, following addition of 5% (composite–soil mass proportion) 1.0 CMC@MMT-FeS. When 2% 0.5 CMC@MMT-FeS was added to Cr(VI)-contaminated soil, the Cr(VI) removal efficiency, as measured in the leaching solution using the toxicity characteristic leaching procedure, was 90.3%, meeting the environmental protection standard for hazardous waste (5 mg/kg). The European Community Bureau of Reference (BCR) test confirmed that the main Cr fractions in the soil samples changed from acid-exchangeable fractions to oxidable fractions and residual fractions after 30 days of soil remediation by the composite. Moreover, the main complex formed during remediation was Fe(III)–Cr(III), based on BCR and X-ray photoelectron spectroscopy analyses. Biotoxicity of the remediated soils, using Vicia faba and Eisenia foetida, was analyzed and evaluated. Our results indicate that CMC@MMT-FeS effectively immobilizes Cr(VI), with widespread potential application in Cr(VI)-contaminated soil remediation.