This study prepared unsupported MoS 2 catalysts by a one-step hydrothermal method using ammonium heptamolybdate and thiocarbamide as materials. The morphology and microstructure of MoS 2 catalysts were changed by adding different amounts of hexadecyl trimethyl ammonium bromide (CTAB). The resultant catalysts were characterized by X-ray diffraction, nitrogen physisorption and transmission electron microscopy. The surface area and pore volume of MoS 2 increased first and then decreased with the addition amount of CTAB. The structural difference between these catalysts lies in the number of layers in stacks and slab length of MoS 2 structure. The structure-activity correlation was studied by using the hydrodeoxygenation (HDO) of p-cresol as the probe reaction. In the HDO of p-cresol, the end products were toluene, 4-methylcyclohexene and methylcyclohexane, and the possible HDO reaction routes were proposed. The effects of addition of CTAB during the synthesis of MoS 2 and HDO reaction temperature on conversion and products distribution were analyzed. The changes of product distribution were explained based on the Rim-Edge model. The direct deoxygenation (DDO) route occurs on the edge active sites while the hydrogenation-dehydration (HYD) route occurs on brim sites of multistacks MoS 2 particles. Thus, the slab length and slab stacking layers had a great effect on the catalytic activity of MoS 2 and products distribution.Electronic supplementary material The online version of this article (