The preparation of LaAlO3 perovskite catalysts for the oxidative coupling of methane (OCM) using a very simple solid-state method with good reproducibility is described. To obtain high performance LaAlO3 catalysts, preparation conditions such as time, temperature, and oxygen content, which have a strong effect on the catalytic activity, are controlled during the calcination process. As the calcination time and temperature increase, the catalytic activity of LaAlO3 improves due to the good homogeneity and high crystallinity of LaAlO3 perovskite. Especially, the LaAlO3 catalyst calcined at 1350 degrees C for 24 h shows the highest selectivity and yield of C-2 hydrocarbons. LaAlO3 catalysts calcined at various oxygen fractions show a volcano-shaped curve with respect to oxygen content in calcination gas, and the LaAlO3 catalyst prepared with an oxygen content of 5 % exhibits the best catalytic performance in this reaction. The appropriate oxygen fraction provides the LaAlO3 catalyst with a large amount of electrophilic lattice oxygen species and a sufficient amount of adsorption oxygen species, which are known to play key roles in the OCM reaction. This study clearly reveals this simple, highly reproducible, and mass-productive solid-state method as a promising preparation method for high performance LaAlO3 perovskite catalysts for OCM.