Using commercial MoS2 as raw material, the exfoliated MoS2 catalyst with a large specific surface area was prepared by adopting n-butyl lithium embedded into the MoS2 crystals. BET, XRD, SEM characterization results showed that the improved preparation method via adding cationic surfactant CTAB into the exfoliation process could reduce the height of the stack layers of MoS2, whereas for the adding of anionic surfactant, the exfoliation effect could not be promoted. The main products for the hydrodeoxygenation of p-cresol by MoS2 catalyst were 4-methylcyclohexene, methylcyclohexane and toluene. The exfoliated MoS2 catalyst had two catalysis activated sites which located at the “Edge” and the “Rim” of the layers of the crstals and [基金项目：国家自然科学基金(No. 21306159, 21376202) *联系作者:杨运泉(1963-)，男，教授，博导,Tel：13055142055，E-mail：yangyunquan@xtu.edu.cn 作者简介: 杨司军(1990-), 男, 湖南省怀化市人, 硕士研究生, 主要从事催化过程及催化新材料研究。 Tel: 15773206350, E-mail:Yangsj900327@163.com]the HDO reaction was much easier to occur at the "Edge". Adding Ni or Co into the exfoliation MoS2 catalyst could improve the activity of HDO and the introduction of Ni could promote the toluene converting into methylcyclohexane, implying that the addition of Ni into the exfoliation MoS2 is more beneficial to the improvement of the fuel oil quality origined from bio-oil raw material. However, the HDO reaction activity of the exfoliated MoS2 was not yet high enough with the addition of Ni or Co into the catalyst, this may be ascribed to the limitation of the specific structure and the chemical activity of MoS2.