As a result of extensive research efforts by several research groups, magnetite-based materials have gained enormous attention in diverse fields including biomedicine, catalysis, energy and data storage devices, magnetic resonance imaging, and environmental remediation. Owing to their low production cost, ease of modification, biocompatibility, and superparamagnetism, the use of these materials for the abatement of environmental toxicants has been increasing continuously. Here we focus on the recent advances in the use of magnetite-based adsorbents for removal of radionuclides (such as 137 Cs(I), 155 Eu(III), 90 Sr(II), 238 U(VI), etc.) from diverse aqueous phases. This review summarizes the preparation and surface modification of magnetite-based adsorbents, their physicochemical properties, adsorption behavior and mechanism, and diverse conventional and recent environmental technological options for the treatment of water contaminated with radionuclides. In addition, case studies for the removal of radionuclides from actual contaminated sites are discussed, and finally the optimization of magnetite-based remedial solutions is presented for practical application.