A template method (alias dictus nanocasting) has been explored for the synthesis of well-defined nanostructured materials. The chemical and physical properties of the obtained nanomaterials can be tuned by the synthesis procedure as well as the precursor materials, and CVD is a powerful method to control nanostructures at the atomic level precisely. For example, Ito and co-workers reported sophisticated macroporous (>50 nm) 3D graphene materials using the CVD of benzene on a porous Ni template. The material maintains the electronic nature of pristine 2D graphene, and its analogs with structural defects, including substitutional defects and adatoms of nitrogen and sulfur, work efficiently as catalyts. owing to their high electrical conductivity. Recently, the effects of structural topology and mechanical and electronic properties have also been well studied. Thus, these materials are excellent candidates for developing ideal 3D graphene materials. However, we recognized that a 3D single-layered graphene architecture with a large pore size and high surface area (>2000 m 2 g -1 ) sometimes collapses the structural regularity of the grown carbons during the template removal process using aqueous acids, as previously reported, leading to stacked carbon layers. Hereafter, we focus on porous graphene analogs with narrow pore distribution (< 20 nm).