We report a simple and efficient approach for fabrication of novel graphene-polysulfide (GPS) anode materials, which consists of conducting graphene network and homogeneously distributed polysulfide in between and chemically bonded with graphene sheets. Such unique architecture not only possesses fast electron transport channels, shortens the Li-ion diffusion length but also provides very efficient Li-ion reservoirs. As a consequence, the GPS materials exhibit an ultrahigh reversible capacity, excellent rate capability and superior long-term cycling performance in terms of 1600, 550, 380 mAh g(-1) after 500, 1300, 1900 cycles with a rate of 1, 5 and 10 A g(-1) respectively. This novel and simple strategy is believed to work broadly for other carbon-based materials. Additionally, the competitive cost and low environment impact may promise such materials and technique a promising future for the development of high-performance energy storage devices for diverse applications.