Three-dimensional (3-D) graphene nanosheet materials are generally divided into two categories: (1) Macroscale materials, where all dimensions are larger than 100 μm, including materials such as foam, sponge, and aerogel; (2) Microscale materials, namely, powders with sizes smaller than 100 μm in each dimension tend to be powders at the macro scale, but have sub–macrocharacteristics at the nanometer-micron scale. The 3-D graphene nanosheet materials can be used as both catalytic active electrodes and conductive 3-D carriers of active materials for electrochemical energy storage and conversion, as well as environmental remediation. In this chapter, the structural features, preparation methods, energy and environmental applications, and typical case analysis of 3-D graphene nanosheet materials are briefly analyzed and summarized.