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In this paper, the preparation and the test of the endothermic properties of modified expanded graphitebased CaxZny(OH)2(x+y) composite materials are reported, which is promised to be used for heat storage. Coprecipitation method is employed to prepare the modified expanded graphite-based CaxZny(OH)2(x+y) composite materials for heat storage. Ca(OH)2 is dissolved in water first, and a certain amount of ZnO is added into the Ca(OH)2 solution to get a milky suspension; thereafter the modified expanded graphite is immersed into the milky suspension to prepare the composite materials by way of physical adsorption. Furthermore, differential scanning calorimetric analyzer is used to analyze the endothermic properties of the material. The results show that the endothermic enthalpy of the composite material is about 1000 J/g with lower decomposition temperature.