Graphene, a two-dimensional carbon sheet with monoatomic layer thickness, has attracted tremendous attention from both theoretical and experimental researchers in recent years. Based on its unique properties, graphene-based materials offer great potential for energy storage. However, for electrochemical energy storage devices application, two main challenges need to be solved urgently. i) Novel graphene-based electrode active materials and new material systems emerged in basic study endlessly, but which can achieve industrial applications are handful. ii) The basic studies on electrode manufacturing process engineering are rarely, process theory is blank for large capacity single cell manufacture. In this report, we will introduce our research strategy for high properties graphene-based energy storage devices. We will summarize our investigation on a series of advanced graphene-based anode materials and systems for lithium ion battery (LIB) application (Figure 1), which hold many favorable advantages including inhibitory restacking and agglomeration of graphene sheets, stable 3D structures, excellent electrochemical performance and beneficial to scale-up application. For graphene sheets (GS) anode, a simple method of filter can prevent the restacking of chemically converted GS by a “spacer” effect of water, which presented a reversible capacity of 645.2 mAh g-1.1 As flexible and free-standing anode, GS films have the potential to improve the energy density of LIB and other energy storage devices. For active material/GS composites anode, the targeted choice of appropriate preparation methods, such as spray-drying,2-4 one-step solvothermal,5 green hydrothermal,6,7 etc, not only can improve the electrochemical performance (e.g. high intrinsic capacity, stable cycling performance and high rate performance) of the active materials, but also benefit for industrial scale up. Finally, the suitable electrolyte system for graphene-based electrode will also be reported. Acknowledgement We are grateful for financial support for this work from the National Basic Research Program of China (2014CB239700), the Natural Science Foundation of China (21336003, 21403139), China Postdoctoral Science Foundation (2013M541510), and the Science and Technology Commission of Shanghai Municipality (14DZ2250800).