The removal of cesium (Cs) from contaminated clay minerals is still a challenge due to the limited efficiency of the process. Thus, this study aimed to enhance the removal for Cs+ ions during the conventional acid washing process by incorporating a bead-type adsorbent. Polyacrylonitrile-based nickel potassium hexacyanoferrate (NiFC-PAN) was utilized as the Cs adsorbent to selectively adsorb Cs+ ions in a strongly acidic solution that contained competing ions. To enable easy separation of clay particles and protect the adsorbent from harsh environmental conditions, PAN was deliberately constructed as large beads. The synthesized adsorbent (NiFC/PAN in a 2:1 ratio) displayed high selectivity for Cs+ ions and had a maximum capacity of 162.78 mg/g for Cs+ adsorption in 0.5 M HNO3 solution. Since NiFC-PAN exhibited greater Cs selectivity than the clay mineral (hydrobiotite, HBT), adding NiFC-PAN during the acid washing substantially increased Cs desorption (73.3%) by preventing the re-adsorption for Cs+ ions on the HBT. The acid treatment in the presence of NiFCPAN also significantly decreased the radioactivity of 137Cs-HBT from 209 to 27 Bq/g, resulting in a desorption efficiency of 87.1%. Therefore, these findings suggest that the proposed technique is a potentially useful and effective method for decontaminating radioactive clay.