The short circuit of cells due to the dissolution and the deposition of NiO in a molten carbonate is a big problem that has to be resolved if we want to use Molten Carbonate Fuel Cells (MCFCs) for long-term operation. To resolve this problem, we have proposed a new cathode structure in which NiO grains have been coated with LiCoO2 grains by usual tape casting method, because LiCoO2 is more stable in a carbonate melt than NiO. CoO/NiO composites with 5 to 20 mass% Ca could be formed by using the CoO/Ni composite particles; As confirmed by SEM, these composites consisted of NiO cores covered with the outer layer of Li(Co, Ni) oxide. The stability of the lithiated CoO/NiO composite with 5 mass% CoO was significantly improved in comparison with that of conventional NiO for MCFCs. The lithiated CoO/NiO composite was also successfully formed by in-situ oxidation and lithiation process. We thought that this composite cathode material consisting of NiO core covered with Li(Co, Ni) oxide will be adopted as the new cathode for MCFCs.