In　this　investigation,　nitrogen　and　sulfur　co-doped　graphene　hydrogel　(N,S-GH)　with　well-connected　hierarchical　networks　was　prepared　using　a　simple　one-step　process.　The　hierarchical　structures　provide　electrically　conductive　channels　for　ion　transfer,　whereas　N,S　heteroatoms　improve　the　chemical　reactivity　and　pseudocapacitance　of　the　electrode　material.　An　optimized　N,S-GH　as　a　bind-free　supercapacitor　electrode　demonstrates　a　large　gravimetric　capacitance　(294.8　F　g(-1)　at　1　A　g(-1)),　long　lifetime　(89.4%　retention　after　10,000　cycles),　and　excellent　rate　capability,　twice　as　that　of　pure　GH　due　to　the　synergistic　effect　of　N　and　S　doping.　Therefore,　a　large　capacitance　of　the　optimized　N,S-GH　is　ascribed　to　fast　ion　diffusion,　large　accessible　area　(hierarchical　network),　and　pseudocapacitance　(N　and　S　co-doping).　Furthermore,　the　optimized　N,S-GH-based　supercapacitor　delivers　a　high　energy　density　(8.6　Wh　kg(-1))　at　a　high　power　density　(2.4　kW　kg(-1)).　Overall,　the　obtained　N,S-GH　through　this　investigation　presents　a　promising　electrode　material　with　outstanding　electrochemical　properties　for　energy　storage　applications.