The development of efficient energy storage materials is crucial to the future renewable energy infrastructure. In this work, molybdenum disulfide/polypyrrole (MoS2/PPy) nanocomposites are synthesized in a facile hydrothermal process, where in situ oxidation polymerization of pyrrole occurs in the presence of MoS2 suspension, for their use as supercapacitor electrodes. The layered MoS2 structure serves as 2D conductive skeleton to facilitate the mobility of protons in and out from the nanocomposites, making it easily accessible and shortening the path length for electrolyte ions transport. Further, the electrochemical performance was evaluated by cyclic voltammogram, electrochemical impedance spectroscopy and galvanostatic charge/discharge, electrochemical stability, Ragone plot and cycling process. The MoS2/PPy electrode exhibits high specific capacitance of 654Fg−1 and significantly retains its 95% performance after 500 cycles at a current density of 3Ag−1significantly higher than its pristine counterparts. The improved performance of the hybrid nanocomposites due to layered MoS2 imparts the necessary space for ions during charge–discharge and stability to polymeric backbone.