Alkylphenols are indispensable chemicals that are currently derived from fossil resources. Conversion of lignin into alkylphenols in a selective manner is highly desirable, while it represents one of the biggest challenges in biorefinery. Herein, lignin depolymerization coupling with methoxy removal over supported MoS 2 catalyst for the direct production of alkylphenols has been studied. The catalysts were prepared by incipient wetness impregnation and characterized by N 2 physisorption, XRD, NH 3 -TPD, CO chemisorption, ICP, TEM, and XPS. The catalytic performance and the reaction mechanism were initially assessed by the hydrodeoxygenation (HDO) of eugenol. Among the catalysts with MoS 2 supported on different supports (HZSM-5, SAPO-34, SiO 2 , Al 2 O 3 , and activated carbon (AC)), the acid-rich MoS 2 /AC with high specific surface areas and more exposed MoS 2 edge sites owed a complete conversion of eugenol and 64.8% yield of 4-propylphenol under 3 MPa H 2 at 300 °C for 3 h. In the conversion of lignin-oil, MoS 2 /AC catalyst also exhibited excellent activity in the removal of all the methoxy groups in various aromatic monomers, achieving alkylphenols with selectivity up to 76.2%. Notably, this catalytic system also showed potential in simultaneous hydrocracking coupling with methoxy removal of realistic lignin to afford alkylphenols, thus providing a direct strategy for the selective valorization of lignin.