ABSTRACT A series of nonstoichiometric compounds K2 xNix/2[NiFe(CN)6]nH2O was prepared by varying Ni/Fe molar ratio from 0.1 to 100. The products had a face-centered cubic (fee) structure, and the lattice parameter slightly increased with decreasing K/Fe ratio. The uptake rate of Cs+ was enhanced at lower K/Fe ratio below 1.32 and reached equilibrium within 8 h for the products with K/Fe below 0.86. The distribution coefficients of Cs+ on the products were above 104 cm3/g in the presence of 1 mol/dm3 Na+, K+ or H+ while those of other nuclides were less than 102, indicating high selectivity of the product to Cs+. The uptake of Cs+ followed a Langmuir-type isotherm and the maximum amount of Cs+ adsorbed was evaluated to be 1.0 to 1.5 mmol/g. Cesium nuclides were efficiently removed from a simulated high-level liquid waste.