In recent years, tremendous research effort has been aimed at increasing the energy density of supercapacitors without sacrificing high power capability so that they reach the levels achieved in batteries and at lowering fabrication costs. For this purpose, two important problems have to be solved: first, it is critical to develop ways to design high performance electrode materials for supercapacitors; second, it is necessary to achieve controllably assembled supercapacitor types (such as symmetric capacitors including double‐layer and pseudo‐capacitors, asymmetric capacitors, and Li‐ion capacitors). The explosive growth of research in this field makes this review timely. Recent progress in the research and development of high performance electrode materials and high‐energy supercapacitors is summarized. Several key issues for improving the energy densities of supercapacitors and some mutual relationships among various effecting parameters are reviewed, and challenges and perspectives in this exciting field are also discussed. This provides fundamental insight into supercapacitors and offers an important guideline for future design of advanced next‐generation supercapacitors for industrial and consumer applications.

This review summarizes recent progress in the design and fabrication of carbon materials for high volumetric performance supercapacitors.

We demonstrated the fabrication of functionalized graphene nanosheets via low temperature (300 °C) treatment of graphite oxide with a slow heating rate using Mg(OH)2 nanosheets as template. Because of its dented sheet with high surface area, a certain amount of oxygen-containing groups, and low pore volume, the as-obtained graphene delivers both ultrahigh specific gravimetric and volumetric capacitances of 456 F g(-1) and 470 F cm(-3), almost 3.7 times and 3.3 times higher than hydrazine reduced graphene, respectively. Especially, the obtained volumetric capacitance is the highest value so far reported for carbon materials in aqueous electrolytes. More importantly, the assembled supercapacitor exhibits an ultrahigh volumetric energy density of 27.2 Wh L(-1), which is among the highest values for carbon materials in aqueous electrolytes, as well as excellent cycling stability with 134% of its initial capacitance after 10,000 cycles. Therefore, the present work holds a great promise for future design and large-scale production of high performance graphene electrodes for portable energy storage devices.

3D pillared‐porous carbon nanosheets with supporting carbon pillars between the carbon layers is prepared by the carbonization of pitch on porous MgO templates. This unique structure endows the high‐rate transportation of electrolyte ions and electrons throughout the electrode matrix, resulting in excellent electrochemical performance.