Catalysis plays a key role in oriented biomass valorization, and designing a robust catalyst and developing its correspondingly easy-to-scale-up preparation are particularly crucial in boosting biorefinery concept into reality. In this study, employing sulfur vacancies in MoS 3 and their preferable adsorption to Co ions, CoS-MoS 2 catalyst was fabricated via decomposition of MoS 3 followed by in situ sulfidation of Co oxides. Co could be located at the edges of MoS 2 , constructing plenty of CoS−edge interfaces. This critical feature of the interface enhanced the adsorption of the reactant and decreased the energy barrier of the rate-limiting step in the deoxygenation of 4-methylphenol, leading to as high as 100% toluene yield at a low temperature of 120 °C. Moreover, this catalyst presented high stability in the deoxygenation reaction and could efficiently convert other lignin-derived aromatic oxy-compounds into arenes. Importantly, this facile method shows good versatility in fabricating different iron family element-promoted MoS 2 -based catalysts, and this preparation procedure is readily scaled up 200-fold without compromising catalytic activity, showcasing the potential for large-scale applications.