Radioactive waste is a byproduct of nuclear power generation and applications of various radioactive materials in many fields. This waste has been strictly regulated as a highly hazardous material to all forms of life and the environment. The technologies currently adopted for managing radioactive waste are mainly based on segregation and storage. Ideally radioactive waste should be isolated from entering the environment, but there has been slow progress toward sustainable waste management. Nanomaterials, with the unique physical and chemical properties, such as nano-size effect, large specific surface area, high reactivity and selectivity, have become a new type of materials for radioactive wastewater decontamination. Therefore, this review aims to provide an comprehensive overview and analysis of the new generation of nanomaterials which have been demonstrated effective for radioactive wastewater decontamination, including carbon-based nanomaterials, metal nanoparticles, nanosized metal oxides, metal sulfides, nano-sized natural materials, layered double hydroxides, hydroxyapatite nanoparticles, metal-organic frameworks, cellulose nanomaterials, biogenic nanocomposites, etc. Although many different types of nanomaterials have been developed, their engineering feasibility toward radioactive wastewater decontamination has not yet been demonstrated at real large-scale applications. Lastly, the challenges associated with the applications of nanomaterials for radioactive wastewater decontamination were discussed in detail, while shedding light on future research direction.