In this study, a series of H-BZSM-5 catalysts, rich in porous structures, were prepared by a template-free method followed by an alkali treatment, each of which was combined with a Zn-ZSM-S catalyst to produce aromatic hydrocarbons from methanol via low-carbon olefins. By separately designing suitable catalysts that satisfy the needs of these two stages, and appropriately matching these two catalysts, the stability of the catalyst and single-pass aromatic production is expected to improve. For two-step coupling to produce aromatic hydrocarbons, the HBZS-x-AT catalyst (H-BZSM-5 treated with NaOH + Al(NO3)(3)) was selected for the conversion of methanol to low-carbon olefins. Adding an appropriate amount of aluminum during the alkali treatment can suppress the over-etching of the silicon-rich region inside the crystal and, at the same time, aluminum atoms and boron atoms undergo isomorphous substitution. While introducing continuous mesopores, some strong acid sites are introduced, significantly improving the stability of B-ZSM-S in the methanol-to-olefin (Step 1) reaction. The HBZS-27-AT catalyst has a suitable catalyst lifetime, high C-2(=)-C-4(=) intermediate product selectivity, with a total selectivity of 73%, which is beneficial to subsequent olefin aromatization. The Zn-ZSM-S catalyst was selected for the preparation of aromatics from low-carbon olefins (Step 2). Considering the effect of the composite method and ratio of the two kinds of catalysts on the performance of the two-step coupled aromatic production, it is concluded that, when the composite catalyst has upper and lower layer filling and the ratio is 3:7, compared with the traditional Zn-modified ZSM-5, the stability of the catalyst was increased from 3 to 194 h, and the single-pass aromatic production increased from 0.15 to 4.98 g/g catalyst.