Abstract: The pyrolysis of distilled residue of lemongrass, which is a traditional Chinese medicine residue, can not only solve the problem of solid waste, but also obtain high-value chemicals, thus achieve the purpose of resource utilization. In this study, Ni-Al layered double oxide/zeolite composite catalyst (NiAl-LDO/ZSM-5) was prepared by using NaOH-treated ZSM-5 as the support, and used in the pyrolysis of lemongrass residue under methanol atmosphere. The catalyst characterization results showed that the ZSM-5 framework was damaged by NaOH treatment, and the degree of damage increased with the increase of the concentration of NaOH solution. After loading NiAl-LDO, the specific surface area of catalyst decreased, but with the increase of NaOH concentration, the specific surface area of catalyst increased gradually as well as the weak acidic sites and the strong acidic sites. The catalytic pyrolysis results showed that the yield of bio-oil obtained by NiAl-LDO/ZSM-5 without NaOH treatment was 13.4%. As NiAl-LDO covered the strong acid sites of ZSM-5, the content of benzenes in the bio-oil increased from 34.06% to 43.15%, and the content of naphthalenes decreased from 63.31% to 23.15%. After the NaOH treatment of ZSM-5 support, the yield of bio-oil was almost unchanged. However, with the increase of the concentration of NaOH solution, the content of aromatic hydrocarbons in the pyrolysis bio-oil increased from 16.35% to 50.19%, and the content of oxygen-containing compounds decreased gradually from 35.35% to 17.38%.