Layered MoS2 with unique structural and electronic properties has received increasing research interest for its potential catalytic properties. It is a challenge to develop strategies to improve the conductivity of MoS2 nanosheets. Here, we report an aluminum decoration on MoS2 ultrathin nanosheets by using the modified atomic layer deposition technique, which shows improved conductivity and enhanced catalytic activity for hydrogen evolution reaction (HER) with overpotentials of 248 and 198 mV that are derived for Al-MoS2 at 10 mA cm–2 in acidic and basic media, respectively. The findings in this work will provide the effective way for modulating the MoS2 with the metallic decorations, which may further advance the development of the 2D material, especially for those with poor conductivity.