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Utilizing lignocellulosic biomass as a renewable energy source for the production of sustainable fuel is of paramount importance. This study focuses on the catalytic co-pyrolysis of Mesua ferrea L. de-oiled cake (MDC) and Garlic husk (GH) as potential feedstocks for bio-fuel production. The pyrolysis experiments were conducted using a semi-batch reactor under inert conditions at temperatures of 500, 550, and 600 °C, with a heating rate of 10 °C min−1, a particle size below 1 mm, and an inert gas flow rate of 80 mL min−1. The findings reveal that temperature significantly influences the yield of pyrolytic products. However, GC-MS analysis detected higher oxygenated compounds in the bio-oil, negatively impacting its heating value. To improve fuel quality, co-pyrolysis with and without a catalyst for a feedstock ratio of 1:1 w/w was performed. Red mud, an alkaline waste mainly composed of Fe2O3, Al2O3, and SiO2, is a hazardous environmental concern from aluminum production and is used as a catalyst. The red-mud catalysts reduced oxygen concentration and increased carbon content, acidity, and heating value in the pyrolytic oil. GC-MS analysis of the bio-oil confirmed that using catalysts combined with MDC and GH significantly decreased the concentration of acidic and aromatic compounds, thereby improving the pyrolytic oil's higher heating value (HHV). [ABSTRACT FROM AUTHOR]