To increase the energy density of supercapacitors to approach that of batteries, the current research is always directed towards the cathode materials, whereas the anode materials are rarely studied. In the present work, single-crystalline Fe 2 O 3 nanoparticles directly grown on graphene hydrogels are investigated as high performance anode materials for supercapacitors. During the formation of the graphene/Fe 2 O 3 composite hydrogels, flexible graphene sheets decorated with Fe 2 O 3 particles are self-assembled to form interconnected porous microstructures with high specific surface area, which strongly facilitate charge and ion transport in the full electrode. Infrared spectra show that hydrogen bond is formed between C–OH on graphene hydrogels and Fe 2 O 3 . Benefits from the combined graphene hydrogels and Fe 2 O 3 particles in such a unique structure are that the graphene/Fe 2 O 3 composite electrode exhibits an ultrahigh specific capacitance of 908Fg −1 at 2Ag −1 within the potential range from −1.05 to −0.3V, and an outstanding rate capability (69% capacity retention at 50Ag −1 ). Furthermore, the cycling performance is clearly much better for the graphene/Fe 2 O 3 composite hydrogels than that for pure Fe 2 O 3 sample. These findings open a new pathway to the design and fabrication of three-dimensional graphene hydrogel composites as anode materials in the development of high-performance energy-storage systems.