Two-step hydrothermal method was developed for the synthesis of NiS2//MoS2 catalysts.
NiS2 and MoS2 existed separately in the resultant catalysts.
NiS2//MoS2 catalyst presented a higher surface area and exposed more active sites.
Both methylcyclohexane selectivity and deoxygenation degree on NiS2//MoS2 catalysts were enhanced.
The hydrodeoxygenation mechanism was well explained by the Remote Control model via spillover hydrogen.