Intelligently magnetic nanospheres with potential-triggered undamaged regeneration ability and super paramagnetism for selective Cs+ separation and recovery are synthesized. Each nanosphere is composed of Prussian blue (PB) with strong Cs+ affinity modified magnetic Fe3O4 (Fe3O4@PB). The magnetic Fe3O4@PB nanospheres show rapid Cesium ion (Cs+) insertion release kinetics, which is attributed to the good affinity of PB toward Cs+ and the large specific surface area. The Cs+ adsorbed nanospheres can be easily regenerated by simply switching potential of magnetic electrode in an electromagnetic coupling regeneration reactor. Excitingly, the Cs+ adsorption capacity is nearly invariable after 20 adsorption-regeneration cycles and a high regeneration efficiency over 99% is maintained in each cycle. The smart regeneration mechanism is clarified by electrochemical experiment and advanced quantum chemistry calculation. This intelligently magnetic nanospheres with potential-triggered undamaged regeneration ability should be a promising alternative materials for selective separation and recovery of metal ions from wastewater. (C) 2017 Elsevier B.V. All rights reserved.