Copper-zeolites have been reported to catalyze the direct conversion of methane to methanol. In this work, we report that pretreatment of copper-mordenite (Cu-MOR) using a gas mixture of NO and NH3 (NO/NH3) results in remarkably increased activity for the direct oxidation of methane to methanol. The methanol yield over the pretreated catalysts reaches as high as 106 Î¼mol/gcat, compared to 28 Î¼mol/gcat over the un-pretreated Cu-MOR. The NO/NH3 gas pretreatment redisperses CuO nanoparticles to Cu ions with catalytically favorable Cu oxidation state.