Hydrothermal post-synthesis was used to modify the micropores and acidity of commercially available HZSM-5 zeolites. The recrystallization and the dynamic incorporation and extraction of the framework Al not only stabilized the framework with high crystallinity, but also inhibited the creation of extra-pores during the post-synthesis in NaOH aqueous solution. The resulted Mo/HZSM-5 catalyst showed rather high catalytic stability and greatly enhanced selectivity towards aromatics for methane dehydroaromatization reaction by effectively inhibiting the coke formation.