In recent years, the development of novel nanogrpahenes have drawn huge interests mainly because of their use in optical, electronic and energy devices. In our lab, we have developed syntheses of a series of 2D and 3D nanographenes with various functional groups attached to the edge of the nanographene basil planes. These nanographenes reveal long and short range orders in their self-assemblies. Such orders can be clearly visualized by high resolution TEM with well defined d-spacing between nanographene layers. These nanographenes are semiconductors with tunable electronic structures and processibility in organic solvents. We have demonstrated their use for optical and electronic devices. Among other potential application, these high-surface area nanographenes have an excellent cyclic durability and a much enhanced charge capacity as novel anode materials for LIBs. Moreover, theoretical charge capacity of these nanographenes exceeds 2000 mAh/g due to an increased edge to surface ratio and oxygen containing functional groups.