With the widespread using of nuclear energy, the nuclear technology is developed rapidly and the radionuclide pollution such as uranium has become the serious problem for human health. Nanoscale Zero-Valent Iron (nZVI) has become the excellent adsorbent for the removal of uranium ions from environment because of its low cost, easy preparation, high surface-activity and excellent performance for adsorption of uranium. Due to synergistic effect of each monomer, the nZVI nanocomposites have been applied to remove radionuclides and the adsorption capacity of nZVI nanocomposites are improved to a further level. Hence, the preparation of nZVI and its nanocomposites for the efficient removal of radionuclides is one of the hot issues in the field of environmental science. The aim of this review is to summarize and outlook the recent research on the application of nZVI nanocomposites for the efficient removal of radioactive uranium from environment. The preparation of nZVI and its composites, the removal efficiency and removal mechanism has been summarized, and the application of the nZVI nanocomposites in environmental pollution cleanup has also been discussed, expecting for the reference of practical application and future research.