For innovative application in wastewater treatment techniques, MnO-Fe2O3 nanocomposites were successfully synthesized using the sol–gel auto-combustion method at different temperatures for the adsorption of 137Cs and 60Co radionuclides from aqueous solution. The characterization of these nanocomposites was carried out through FT-IR, SEM-EDX, and X-ray diffraction. These nanocomposites were employed as adsorbent materials for the removal of 137Cs and 60Co radionuclides from simulated radioactive waste solutions. The study involved a series of experiments aiming to demonstrate the MnO-Fe2O3 nanoparticles’ exceptional adsorption potential concerning 137Cs and 60Co. Additionally, the investigation delved into how variations in temperature, dose amount, contact time, and pH value influence the adsorption dynamics. Due to their high specific surface area, the synthesized MnO-Fe2O3 nanoparticles had high adsorption capacity of more than 60% and 90% for 137Cs and 60Co, respectively. By investigation of kinetics and adsorption isotherms, pseudo-second-order reaction and the Langmuir model turned out to fit well for the adsorption of 137Cs and 60Co onto the MnO-Fe2O3 nanocomposites. Moreover, a thermodynamic analysis revealed that the adsorption process was spontaneous for both target metals and the adsorption of 60Co was endothermic, whereas the adsorption of 137Cs was exothermic.