The electrocatalytic performance of MoS2 material is largely restricted by its electrical conductivity and acid-base environment. Therefore, it is necessary to improve the surface activity and widen its pH range in actual application. In this work, we design Fe-MoS2@PPy nanosheet structures by combining hydrothermal and electrodeposition routes. The introduction of Fe ions expands the lattice of MoS2 phase, which provides many active sites for the hydrolysis of water. PPy film is beneficial to the electrical conductivity and chemical performances of the catalysts. The overpotentials of hybrid Fe-MoS2@PPy-5 electrocatalyst is 217, 193 and 164 mV in 1 M PBS, 0.5 M H2SO4 and 1 M KOH electrolytes, respectively. The enhancement in HER performance and excellent long-term stability occurred because of strong electronic interactions between the Fe-MoS2 and PPy, which promotes the electrical conductivity and prohibiting the dissolution of electrocatalysts. This synthesis strategy can be used to prepare other transition metal compound electrocatalysts under all pH value condition.