The modified surface of activated carbon (MSAC) was prepared from the agricultural byproduct coconut shells, by physical and chemical activation processes, and it was tested for the treatment of simulated radioactive waste solutions included some metal ions, namely Europium, Cerium, Strontium, and Cesium. The structural morphology and composition of the modified surface activated carbon coconut shells (MSAC) were evaluated by SEM, XRD, FTIR, XRF, and elemental analysis. The solubility experiments show that the prepared sorbent (MSAC) has reasonably good chemical stability. The influence of solution pH, contact time, adsorbent dosage, adsorption temperature, initial metal ion concentration and interfering substances such as sodium chloride salt and ethylenediaminetetraacetic acid (EDTA), on the adsorption performance of Eu³⁺, Ce³⁺, Sr²⁺ and Cs⁺ ions on to the prepared sorbent (MSAC)  were examined by batch technique. The saturation capacity of the MSAC for the studied metal ions was  found to be very high as compared to the break-through capacity, and it was found to be 136.84, 85.55, 69.85 and 60.00 mg g ^-1 for Eu³⁺, Ce³⁺, Sr²⁺ ,and Cs⁺ ions, respectively. Using the Van^,t Hoff  linear plot, the thermodynamic parameters, ΔH^o, ΔS^o ,and ΔG^o were also evaluated. . Results show that studied sorbent (MSAC) is efficient to remove more than 98.43, 90.7, 38.65, and 37.4%, of Eu ^3+, Ce ^3+, Sr ²⁺ and Cs ⁺ ions respectively, at 180 min equilibrium time. The developed sorbent is considered as a good replacement technology for removal of Eu³⁺, Ce³⁺, Sr²⁺ ,and Cs⁺ ions from radioactive waste solutions due to its low-cost , good efficiency, high saturation capacity, as well as easy handling with no or small amount of secondary sludge.