Acid reflux-dealuminated HMCM-22 supported Mo catalyst exhibits highly selective and coking-resistant catalytic performance for methane dehydrocondensation reaction, compared with conventional catalysts. The excellent catalytic stability of the dealuminated catalyst is based on the remarkable suppression of coke formation owing to the effective decrease of Bronsted acid sites, which are demonstrated by TPO, H-1 NMR and NH3-TPD methods.