Diopside is known to be a ceramic phase with excellent thermal properties (~2.7 W/mK), but the thermal conductivity is not high enough to apply it as a LED packaging material. The chip and PCB (printed circuit board) will deteriorate if the heat is not released out of the LED device. In this study, glass-frit CaO-MgO-SiO2 systems with a stoichiometric diopside phase composition containing ZnO of various types and amounts were fabricated. The thermal conductivity, density, and shrinkage as a function of the type of ZnO added were studied to investigate the feasibility of utilizing diopside-based glass ceramics in LED packaging applications. It was found that at temperatures below 1000℃, it is possible to fabricate diopside/ZnO composites with thermal conductivity values of approximately 5.7 W/mK, 2.1 times higher than that of pure diopside, by adding single-crystalline ZnO filler to the mother glass. The diopside/ZnO composites fabricated in this study can therefore be applied to LED packaging materials. They are also suitable for the LTCC process.