This study explores the application of graphene quantum dots (GQDs) as innovative nanomaterials for the efficient removal of nuclear materials from metal and plastic surfaces, especially in contexts involving terrorist threats, such as “dirty bombs” and radiological dispersal devices (RDDs). These devices use conventional explosives combined with radioactive materials to contaminate large areas, posing significant risks to health and the environment. This investigation addresses the growing global concern about the use and threat of such weapons, particularly in the context of escalating wars and the increasing vulnerability of nuclear facilities to security breaches. Our focus is on the unique properties of GQDs—such as their chemical stability, high surface area, quantum confinement effects, and electronic characteristics—that enhance their ability to effectively adsorb radioactive isotopes. We examine the potential of GQDs to interact with various radioactive materials, focusing on isotopes commonly associated with RDDs, such as cesium-137, cobalt-60, strontium-90, and iridium-192. Functionalization techniques are employed to enhance the interaction of GQDs with specific isotopes, thus improving the decontamination process. Our findings reveal that GQDs can efficiently remove iodine-131 (I-131) from several metals: Aluminum (91.27%), zinc (98.67%), and monel (96.40%). They also demonstrate high efficiency in removing I-131 from rigid polyvinyl chloride. On the other hand, GQDs presented moderate efficiency in removing technetium-99m, with removal rates of 64.93% from monel, 55.11% from aluminum, and 41.80% from zinc. Overall, GQDs could play a crucial role in mitigating the consequences of dirty bomb detonations, offering a quick and effective method to reduce radiological impacts in affected areas. This research enhances our understanding of nanomaterials in responding to radiological emergencies, presenting GQDs as a viable solution to contemporary challenges in public health and safety. The implications of this study extend beyond immediate decontamination, suggesting broader applications of GQDs in environmental safety and nuclear safety protocols.