Hydrocarbon generating and expulsion simulation experiments are carried out using samples artifically matched between the acid-dissolved residue of relatively low-maturity limestone and the original sample. This work makes up for the insufficiency of source rock samples with high abundance of organic matters and low maturity in China. The organic carbon content of the 10 prepared samples varies between 0.15% and 0.74%. Pyrolysis data and simulation experiment results of hydrocarbon generating and expulsion, which were obtained by a high-temperature and high-pressure open system, indicate that the lower limit of organic carbon content for marine carbonate rock to generate and expel hydrocarbons is 0.23%—0.31%. In combination with the numerical analysis of organic carbon in marine carbonate rocks from Tarim Basin, Sichuan Basin, Ordos Basin and North China, as well as the contribution of these gas source rocks to the discovered gas pools, we think that the organic carbon criterion for carbonate gas source rocks should be 0.3%.