Abstract: The present invention is related to a method of coupling methane dry-reforming and composite catalyst regeneration. A composite catalyst is filled into a reactor, and methane or a methane mixture gas is introduced therein. CaCO3 in the composite catalyst is decomposed under 600-850° C. CO2 obtained by the decomposition reacts with methane to perform methane dry-reforming reaction and produce synthesis gas containing CO and hydrogen. The composite catalyst contains CaCO3 , active nickel and alumina support. This method couples the CaCO3 decomposition reaction in calcium looping and methane dry-reforming reaction to solve the technical problem of limiting CaCO3 decomposition by high-temperature equilibrium. The decomposition of CaCO3 is enhanced, and the CO2 produced by decomposing CaCO3 is dry-reformed to produce synthesis gas to be utilized.