( )Improving the C-2+ alcohols selectivity is highly desirable for higher alcohols synthesis in CO hydrogenation. Herein, an effective method was developed for Mo-based supported catalysts by the combination of tungsten-doping and surfactant-assisted hydrothermal strategy. The tungsten-doping enhanced the interaction between Ni and W/Mo metal species to form more of the Ni-MoW-S phase with tunable slab size and stacking layers, and thus promoted the chain growth of alcohol to form a greater amount of higher alcohols in CO hydrogenation. The optimal K,Ni - Mo0.75W0.25/MMO-S exhibited a dominant double-layer structure (similar to 39.0%) and highly synergetic effects between Ni and W/Mo species, resulting in the highest total alcohol selectivity (76.1%) and in higher alcohols selectivity. This work provides a new route for tuning the morphology of MoS2/WS2 and synergetic effects between Ni and W/Mo species in supported catalysts to improve the selectivity of higher alcohols.