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The TSR process may be one of the reasons to result in the natural gas destruction in deep carbonate reservoirs. The work on this field has been the subject of much research in recent years. In this paper, thermal simulation experiments on the reaction of CH 4 -CaSO 4 were carried out using autoclave at high temperature and high pressure. The products were characterized by some advanced analytical methods. The thermodynamics and kinetics were discussed and the reaction mechanism was investigated tentatively. It is found that the reaction can proceed spontaneously to produce H 2 S, H 2 O and CaCO 3 as the main products at the temperature range of 550―700℃. The activation energy and geological reaction rate calculated from the kinetic model can be compared with those from previous work. The results obtained in this paper can provide important information on the explanation of geochemical depth limit for natural gas and on the exploration of gas reservoirs.