Given the massive interest and rapid developments in graphene research, scientists are now convinced that the controlled preparation of graphene-based materials with hierarchical and well-defined structures will pave the way for achieving high-performance applications of graphene in various technological fields such as optoelectronics, energy storage, polymer composites and catalysis. Self-assembly techniques have become some of the most effective strategies for this purpose. Although 2D self-assembly of graphene has been studied extensively from the perspectives of fundamental research and commercial applications, 3D self-assembly of 2D nanoscale graphene into functional macrostructures with well-defined networks remains as a great challenge and represents an important hurdle towards practical applications. Researchers in China have now provided a solution to this problem by demonstrating the successful preparation of self-assembled graphene hydrogel via a one-step hydrothermal process.