Bifunctional catalysis coupling CO2 to methanol and methanol to hydrocarbons is a promising strategy for the direct hydrogenation of CO2 into high-value chemicals. However, bifunctional catalysts suffer from low productivity due to the inertness of CO2 and high activation energy of C–C coupling. Herein, we report a highly active bifunctional catalyst consisting of ZnO–ZrO2 aerogel and zeolite H-ZSM-5 for the hydrogenation of CO2 into aromatics with 76% selectivity at single-pass CO2 conversion of 16%. The selectivity of CH4 is lower than 1% at the same time. The space time yield of aromatic hydrocarbons is as high as 0.24 g goxide–1 h–1 under the reaction conditions of 340 °C and 40 bar over ae-ZnO–ZrO2/H-ZSM-5 catalyst, which outperforms the previously reported catalysts including modified Fischer–Tropsch catalysts. We demonstrate that the ZnO–ZrO2 aerogel catalyst, which is prepared by a combined sol–gel and subsequent supercritical drying method, not only possesses high surface area but also provides large amount of oxygen vacancies. The formation rate of methanol intermediate over ZnO–ZrO2 is dominated by the total amount of oxygen vacancies. Moreover, the stable performance of bifunctional catalyst at industrially relevant conditions suggests promising prospects for industrial applications.