Direct conversion of syngas to aromatics is an extremely challenging target due to the complex reaction pathways. Herein, we present a well‐designed bifunctional catalyst composed of Mo‐doped ZrO2 nanoparticles and zeolite H‐ZSM‐5 for one‐step conversion of syngas to aromatics. The Mo−ZrO2 converts syngas to methanol as reaction intermediate, which can be successively converted to aromatics by H‐ZSM‐5. Hydrogenation ability of mixed oxides is pivotal to both selectivity and productivity of aromatics. We intensively clarify the individual role of catalyst components among CO activation, H2 activation and aromatization. With a Mo/Zr molar ratio of 1 : 68, the Mo−ZrO2/H‐ZSM‐5 resulted in 76 % selectivity of aromatics at 22 % CO conversion, and the productivity of aromatics reached 0.17 g gcat−1 h−1 at 400 °C and 4 MPa. Moreover, the distribution of aromatics can be tuned by surface modification of H‐ZSM‐5.