Iodine-131 is increasingly used for diagnostic and therapeutic applications. The excretion of radioactive iodine is primarily through the urine. The safe disposal of radioactive waste is an important component of overall hospital waste management. This study investigated the feasibility of using graphene oxide/chitosan (GO/CS) sponges as an adsorbent for the removal of iodine-131 from aqueous solutions. The adsorption efficiency was investigated using iodine-131 radioisotopes to confirm the results in conjunction with stable isotopes. The results revealed that the synthetic structure consists of randomly connected GO sheets without overlapping layers. The equilibrium adsorption data fitted well with the Langmuir model. The separation factor (RL) value was in the range of 0–1, confirming the favorable uptake of the iodide on the GO/CS sponge. The maximum adsorption capacity of iodine-131 by GO/CS sponges was 0.263 MBq/mg. The highest removal efficiency was 92.6% at pH 7.2 ± 0.2. Due to its attractive characteristics, including its low cost, the ease of obtaining it, and its eco-friendly properties, the developed GO/CS sponge could be used as an alternative adsorbent for removing radioiodine from wastewater.