Adamantane was synthesized by the batch reactor system in the presence of hydrogen using endo-tetrahydrodicyclopentadiene (endo-TCD) as reactant,solid super-acid ZrO₂-SO^2－_４(SZ) loaded REY,USY,Si-MCM-41molecular sieves as isomerizing catalysts. Loading ZrO₂-SO^2－_４ on surface of molecular sieve was helpful to increase the yield of adamantane. The effects of reaction temperature,hydrogen pressure,the content of the surface loaded ZrO₂ and the types of molecular sieves on synthesis of adamantane were investigated respectively. The results show that higher temperature(＞270 ℃) will increase the yield of hydrocracking by-products which led to the decrease of adamantane yield. The highest yield of adamantane (22.77%) was obtained by using SZ（20%）/REY as isomerizing catalyst under the following conditions: catalyst/reactant(m/m) is 0.625，reaction temperature is 250 ℃，hydrogen pressure is 1.5 MPa，reaction time is 3 h. The total selectivity of adamantane and exo-TCD was as high as 95%.