Present study, first time we developed a nano-Fe/Ca/CaO dispersion mixture based remediation and volume reduction method of real radioactive cesium contaminated soils. After soil samples treated with 10wt% of nano-Fe/Ca/CaO dispersion mixtures, emitting radiation intensity was reduced from 4.00 μSv/h to 0.95 μSv/h in non-magnetic fraction soils. While, after treatment, about 30wt% magnetic and 70wt% nonmagnetic fraction soils were separated, and it’s condensed radioactive cesium concentration was about 80% and 20%, respectively. By this way, cesium contaminated soil volume can be reduced. These preliminary results appear to be very promising and the simple mixing with the addition of nano-Fe/Ca/CaO may be considered potentially applicable for the remediation and separation of radioactive Cs contaminated soil in dry conditions.