The HDS activity and stability of Ni-Mo2C/AC catalysts, prepared by carbothermal hydrogen reduction (CHR) at different temperatures and with different Ni:Mo ratios, is reported. The highest HDS activity occurred for catalysts with Ni:Mo ratios of 0.38 and 0.19, when prepared at the relatively low CHR temperature of 550 and 600°C, respectively. Partial sulfidation of the Ni-Mo2C/AC catalysts occurred rapidly upon reaction in 2wt% dibenzothiophene (DBT) at 350°C and 2.1MPa H2. Uptake of S was enhanced with increased Ni content, resulting in the formation of Mo2C-MoS2 core-shell structures. The stack height of the MoS2 shell increased with increased Ni content and promoted the direct desulfurization of DBT.