A magnetic filter-continuous electrodeionization (CEDI) hybrid separation system was investigated for the purification of the primary coolant in a nuclear power plant. A magnetic filter system with a 3000 Gauss magnetic field and a CEDI system with a cell consisting of 3 compartments were used for the removal of magnetite and nickel ions, respectively. The hybrid separation system achieved removal rates of 98% for magnetite and 99% for the nickel ions demonstrating its feasibility for the purification of primary coolant.