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Thermal batteries have been used for many military applications such as missiles and ordnance devices. As the thermal battery is composed of anode, cathode, MgO based-molten salt electrolyte and additional heat source, its specific energy density is lower than those of commercial batteries.    By means of substituting MgO based-electrolyte to increase energy density of thermal batteries, we have indentified various ionic solid electrolytes such as LLT(La0.5Li0.5TiO3), LSTZ(Li3/8Sr7/16Ta3/4Zr1/4O3) and LLZ(Li7La3Zr2O12).     As a ruslt, we found out that the LLZ with additivies, Ca and Nb, presents not only excellent ionic conductivity but also stable discharge characteristics at high temperature(≈ 300oC). Additionally, we have verified that the LLZ solid electrolyte is suitable for the full scale of thermal batteries with high energy density.