Potassium copper hexacyanoferrate (KCuHCF)-incorporated magnetic chitosan beads (HMC) were synthesized for both selective Cs+ removal in aqueous solutions and facile recovery of the spent adsorbent. To disperse and immobilize large amounts of the KCuHCF, methyl acrylate and diethylenetriamine were sequentially grafted onto the one-step synthesized magnetic chitosan beads. The additional introduction of amino functionality led to the enriched Cu2+ ions on the bead surface to incorporate KCuHCF into the grafting matrix. Consequently, the HMC exhibited a high Cs+ capacity calculated to be 136.47 mg g−1 from the Langmuir model, and the equilibrium was established within 4 h. Moreover, the HMC exhibited excellent stability in a wide pH range from 4 to 11 and an outstanding Cs+ selectivity (>97%) in seawater (1.11 mg L−1 Cs+). From a practical point of view, the HMC was stable during five successive adsorption cycles and easily recovered by magnets, enabling continuous operation to decontaminate a large volume of wastewater.