The present work is an attempt to optimize the proportion of H-ZSM-5 and Al-MCM-41 in the catalyst mixtures for lignocellulose biomass catalytic pyrolysis. The H-ZSM-5 proportions of 50.0, 66.7, 75.0, and 87.5 wt.% were examined for the upgrading of biomass pyrolysis vapors in the fixed bed reactor. The catalyst mixture of 87.5 wt.% H-ZSM-5 and 12.5 wt.% Al-MCM-41 was found most effective in this study, giving a 65.75% deoxygenation degree. An organic-rich bio-oil was obtained with 74.90 wt.% of carbon content, 8 wt.% of hydrogen content, 15 wt.% oxygen content, a 0.39 wt.% water content, and a high heating value of 34.15 MJ/kg. The highest amount of desirable compounds among the studied catalytic experiments, which include hydrocarbons, phenols, furans, and alcohols, was obtained with a value of 95.89%. A significant improvement in the quality of bio-oil with the utilization of H-ZSM-5 and Al-MCM-41 catalyst mixtures was the rise of desirable compounds in bio-oil.