This study aims to improve the quality and yield of bio-oil produced from ex-situ catalytic pyrolysis of lignocellulosic biomass (sawdust) using a combination of stage catalysts with Al-MCM-41, HZSM-5, and ZrO2. The research employed various methods, including thermogravimetric analysis (TGA), differential scanning calorimetry, bench-scale experiments, and process simulations to analyze the kinetics, thermodynamics, products, and energy flows of the catalytic upgrading process. The introduction of ZrO2 enhances the yield of monoaromatic hydrocarbons (MAHs) in heavy organics. Compared with the dual-catalyst case, the MAHs yield escalates by approximately 344% at a catalyst ratio of 1:3:0.25. Additionally, GC-MS data indicate that the incorporation of ZrO2 promotes the deoxygenation reaction of the guaiacol compound and the oligomerization reactions of PAHs. The integration of ZrO2 as the third catalyst enhances the yield of heavy organics significantly, achieving 16.85% at a catalyst ratio of 1:3:1, which increases by nearly 35.6% compared to the dual-catalyst case. Also, the addition of ZrO2 as the third catalyst enhanced the energy distribution in heavy organics. These findings suggest that the combination of these catalysts improves the fuel properties and yields of the bio-oil.