Radionuclide-contaminated water is carcinogenic and poses numerous severe health risks and environmental dangers. The activated carbon (AC)-based adsorption technique has great potential for treating radionuclide-contaminated water due to its simple design, high efficiency, wide pH range, quickness, low cost and environmental friendliness. This critical review first provides a brief overview of the concerned radionuclides with their associated health hazards as well as different removal techniques and their efficacy of removing them. Following this overview, this study summarizes the surface characteristics and adsorption capabilities of AC derived from different biomass precursors. It compares the adsorption performance of AC to other adsorbents, such as zeolite, graphene, carbon nano-tubes and metal–organic frameworks. Furthermore, this study highlights the different factors that influence the physical characteristics of AC and adsorption capacity, including contact time, solution pH, initial concentration of radionuclides, the initial dosage of the adsorbent, and adsorption temperature. The theoretical models of adsorption isotherm and kinetics, along with their fitting parameter values for AC/radionuclide pairs, are also reviewed. Finally, the modification procedures of pristine AC, factors determining AC characteristics and the impact of modifying agents on the adsorption ability of AC are elucidated in this study; therefore, further research and development can be promoted for designing a highly efficient and practical adsorption-based radionuclide removal system.