Polyoxometalates (POMs) represent a class of nanomaterials, which hold enormous promise for a range of energy-related applications. Their promise is owing to their “special” structure that gives POMs a truly...

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Supercapacitors (SC) are a key technology in energy storage systems, which have attracted extensive attention due to the significant recent breakthroughs in their use in modern wearable and consumer electronics. However, for obtaining a high specific capacitance and rate performance, a cogent design and synthesis of the electrode material with abundant active sites are critically important. Unique three-dimensional (3D) open-porous architectures, composed of thin nanosheets of graphene, can offer fast electron transfer and large electrochemically active surface areas, which makes them promising electrode materials for SCs. Moreover, the electronically conductive framework of the graphene building blocks could deliver excellent specific capacitances, high rate performance, and long-term cycling stability. In this chapter, we provide a structure–property-perfomance relationship of graphene, followed by a discussion of the recent advances in developing exotic 3D graphene macrostructures. Finally, we describe the use of these 3D graphene macroarchitectures to realise SCs with unprecedented performance.