Since the proposal of Mackay crystals, several carbon materials have been reported to achieve high surface areas, structural regularity, and functionality. ZTCs are a class of carbon materials with highly ordered 3D structure and a high specific surface area, while NPGs are extraordinary pluripotent materials with high electrochemical stability owing to fewer electrochemically active edges, high electrical conductivity of up to 18 S cm -1 because of seamless and 3D-developed single graphene sheets, and highly flexible mechanical structure with a bulk modulus of less than 1 GPa. We investigated a general strategy for synthesizing high-quality and continuous 3D nanographene materials using CH4-CVD on nanosized oxide surfaces, where the least stacking of nanographene was achieved to ensure a high surface area with suppressed edge sites. Further investigation will expand the scope of template materials, including ordered oxides 101,103 for synthesizing innovative 3D porous graphene materials in due course. However, challenges remain in achieving better homogeneity of nanographene growth and control of hierarchical structure for better applications. As for 2D graphene Fig. (a) Schematic of new refrigeration system based on the flexible deformation of ordered nanoporous graphene materials 152 upon pressurization, and (b) time-course of gas-phase pressure and temperature on the surface of the materials. growth, 153,154 better control of CVD chemistry by suitable surface catalysis 101,155 including well-controlled defects and dispersed metal-containing reactive sites coupled with computational chemistry 156,157 will be crucial for better 3D graphene materials toward minimal surface graphene. A comprehensive understanding of the structure of NPGs has been one of the central issues in this field. Recent progress in the advanced characterization of carbon materials has accelerated our understanding and control of the nanostructure of advanced carbon materials. We addressed the qualification and quantification of surface defects in NPGs by TPD and Raman spectroscopy, 159-161 whereas Poisson statistics are useful for quantitatively determining the distribution of graphene layers in continuous 3D graphenes. The complementary and convincing direct observation of defects by electron microscopic techniques will result in a much deeper understanding of the nanostructure. These insights into the atomic level structure of NPGs including the chemical and topological defects will be conducive to further control of the high-quality NPGs. Advanced characterization, including computational 168,169 and experimental (Raman spectroscopy, angle-resolved photoemission spectroscopy, X-ray absorption fine structure spectroscopy, 171,172 electron energy loss spectroscopy, 173 X-ray photoelectron spectroscopy, 171 steady-state absorption spectroscopy, and neutron diffraction 174 ) approaches (Fig. ), will provide a more sophisticated understanding and control of novel 3D graphene materials at the atomic level.