This study evaluated the synthesis of optimal materials for high efficiency adsorption and removal characteristics of Cs-137 for radioactive contaminated water, and considered thermal treatment methods to stabilize the spent adsorbent generated after treatment. We synthesized a composite adsorbent with a combination of impregnating metal ferrocyanide that improves the selectivity of Cs adsorption with zeolite capable of removing Cs as a support. The Cs removal efficiency of the composite adsorbent was evaluated, and the stability change of Cs according to the high-temperature sintering was evaluated as a stabilization method of the spent adsorbent. The metal ferrocyanide content of the adsorbent was in the range of 11.8~36.0%. The adsorption experiments were performed using a simulated liquid waste to have a total Cs concentration of 1 mg/L while containing a trace amount of Cs-137, and then gamma radioactivity was analyzed. In order to evaluate the stabilization of the spent adsorbent, heat treatment was performed in the range of 500~1,100°C, and the volatilization rate of Cs during heat treatment and the leaching rate of Cs after heat treatment were compared. In the adsorption experiment, the Cs removal efficiency was higher than 99%, regardless of the amount of metal ferrocyanide in the composite adsorbent. In the sintering experiment on the spent adsorbent, it was confirmed that there was no volatilization of Cs up to 850°C, and then the volatilization rate increased as the heating temperature increased. On the other hand, the leaching rate of Cs in the sintered adsorbent tends to significantly decrease as the heating temperature increases, so that Cs can be stabilized in the sintered body. In addition, as the content of metal ferrocyanide increases, the volatilization rate of Cs rapidly increases, indicating that the unstable metal ferrocyanide in the adsorbent may adversely affect the removal of Cs as well as the thermal treatment stability.