A new reaction mode, i.e., the combined single-pass conversion of methane via oxidative coupling (OCM) over mixed metal oxide (SLC) catalysts and dehydroaromatization (MDA) over Mo/HZSM-5 catalysts, is reported. With the assistance of an OCM reaction over SLC catalysts in the top layer of the reactor, the deactivation resistance of Mo/HZSM-5 catalysts is remarkably enhanced. Under the selected reaction conditions, the CH4 conversion decreased from similar to18 to similar to1% and the aromatics yield decreased from 12.8 to 0.1%, respectively, after running the reaction for 960 min on both 6Mo/HZSM-5 and SLC-6Mo/HZSM-5 catalyst system without O-2 in the feed. On the other hand, for the SLC-6Mo/HZSM-5 catalyst system with O-2 in the feed, the deactivation was improved greatly, and after 960 min onstream the CH4 conversion and aromatics yield were still as high as 12.0 and 8.0%, respectively. The promotion effect mainly appears to be associated with in situ formation of CO2 in the OCM layer, which reacts with coke via the reverse Boudouard reaction.