Different mass ratios of polypyrrole (PPy) to graphene hydrogel (GH) nanocomposites were synthesized by hydrothermal reduction of graphene oxide and chemically oxidative polymerization of pyrrole, forming a three-dimensional framework of PPy wrapped on the surface of GH without adding any toxic reductive agents. Electrochemical tests show that PPy/GH15 nanocomposite exhibits unique electrochemcial properties, such as enhanced electrolytic permeability and high electric capacity. Thanks to the synergistic effect of the pseudo-capacitance of PPy and the electric double layer capacitance of GH, PPy/GH15 exhibits a high specific capacitance of 375Fg−1 at a scan rate of 10mVs−1. In addition, the PPy/GH15 electrode shows good cycling stability, and its specific capacitance retention is 87% even after 4000 charge–discharge cycles in the potential window of −0.1 to 0.6V, suggesting it an ideal electrode material for supercapacitor.