Graphene-based hybrid materials are highly attractive for various applications, particularly as electrode for energy storage devices.However, for developing high performance electrode materials, one has to understand as much as possible the relationship between material structures and their electrochemical properties.With this regards, rational design of the structures and functions of the material is critically important.Aromatic graphenal polymers with rich benzene rings and carbon density are one class of important materials for the development of various well-defined graphene-based materials which are highly attractive as electrode for lithium ion batteries and supercapacitors.