Abstract: With the development of human society, radioactive uranium mining and the relative radioactive pollution is becoming the main problem to environmental pollution protection. Efficient removal of radionuclides from environment is one of the most important issues from biological and environmental point of view. Due to the large specific surface area and high number of active sites, nanoscale zero valent iron(nZVI) materials enhance the remediation efficiencies of radioactive contaminants remarkably. The aim of this review is to show the excellent removal capacity and environmental remediation of nZVI-based materials for radionuclides. A brief introduction on frequently-used nZVI-based materials (e.g., surface modified or porous material supported nZVI materials) and their application in the removal of radionuclides and an exploration of their underlying interaction mechanisms (e.g., adsorption, reduction and oxidation) are presented. In the end, a summary and outlook are also briefly addressed. This review intends to provide deep insight into the design of high performance nZVI-based materials for the potential elimination of radionuclides from aqueous solutions during environmental pollution cleanup.