In Fukushima NPP-1, large amounts of high-activity-level water (HALW) accumulated in the reactor, turbine building and the trench in the facility is treated by circulating injection cooling system. The development of highly functional adsorbents and stable solidification method contributes to the advancement of the decontamination system and environmental remediation. The present study deals with (1) preparation of insoluble ferrocyanide loaded zeolites, (2) selective uptake of Cs+ in seawater, (3) estimation of Cs immobilization ratio and stable solidification. Various kinds of Cs-selective composites loaded with insoluble ferrocyanides (CoFC, NiFC) into the zeolites (zeolite A (A51, A-51J), zeolite X (LSX), chabazite (modified chabazite) and natural mordenite (SA-5)) matrices have been prepared using successive impregnation/precipitation methods by Tohoku University. As for Cs+ adsorption, these composites had relatively large uptake (%) above 95%, distribution coefficients (Kd) above 103 cm3/g and excellent adsorption kinetics even in seawater. The immobilization ratio (%) of Cs for the CoFC saturated with Cs+ was estimated at different calcination temperatures up to 1,200°C in advance. The immobilization ratio was less than 0.1% above 1,000°C, indicating that the adsorbed Cs + ions are completely volatilized and insoluble ferrocyanides had no immobilization ability for Cs. In contrast, the insoluble ferrocyanide-loaded zeolites had excellent Cs immobilization ability; in the case of insoluble ferrocyanide-loaded natural zeolites (NiFC-SA-5, CoFCmodified chabazite), the immobilization ratio was above 99% and 96% even after calcination at 1,000°C and 1,100°C, respectively, indicating that nearly all Cs ions are immobilized in the sintered solid form. On the other hand, the immobilization ratio for the insoluble ferrocyanide-loaded A and X zeolites (NiFC-A (A51, A51J), NiFC-X) tended to decrease with calcining temperature; for example, the immobilization ratio for NiFC-X at 1,000°C and 1,100°C was estimated to be 74.9% and 55.4%, respectively, and many spots concentrating Cs were observed on the surface. The difference in immobilization behavior between natural zeolites and synthetic ones is probably due to the phase transformation and surface morphology at higher temperature above 1,000°C. The stable solidification of insoluble ferrocyanides was thus accomplished by using the excellent Cs immobilization abilities of zeolite matrices (Cs trapping and self-sintering abilities).