With unique structure and excellent properties, nano carbon composites like carbon nanotube (CNT) and graphene (GE), have become research focus in nano technology and nano materials, and promoted the rapid development of multifunctional nanocomposites since their discovery. However, with traditional preparation method, the volume of nanometer carbon content in composite materials can only reach 5%–10% due to nanoparticles aggregation and rheological properties of resin, etc. Different from a small amount of nano carbon reinforced polymer composites, nano carbon composites with high concentrations can better exhibit the properties of nano materials, with more advantages in stress transfer, higher shear and tensile breaking strength, have attracted more and more attention in research and applications for these years. With the development of new nano carbon composite materials, more requirements about the structure design and functional development of materials were put forward. The structure of nano carbon units and their arrangement, uniform dispersion and interfacial interaction are extremely important to performances of composite materials. Traditional way can optimize orientation degree and improve packing density but it is still not enough, such as stretching can effectively improve the mechanical and electrical properties of materials, but cannot fundamentally solve the aggregation phenomenon of nanometer unit, performance of conversion efficiency in nano unit is still low. Fortunately, the nature provided us a new clue on the design of high performance and multifunctionalities of nano carbon materials. Structure and interface bonding composites in the organism are both strong and tough. Therefore, nano carbon composite materials of bionic structure are one of the important development directions in the future, and have got the attention of the researchers. In addition, the bionic structure and interface on the energy conversion phenomena, can also realize the function of the composite material bionic, making the nano carbon composite materials have perception, adaptive, self-driven bionic multi-functional characteristics, etc. First, based on traditional processing methods, we obtained the further optimization of carbon nanotubes orientation degree through bionic processing, with good control of aggregation in high volume content of carbon nanotube composites. Second, the rich interface bonding mechanism in laminated shell structure was found, and a hard and soft material with a certain strength and toughness was prepared. Third, on the basis of functional bionics, more abundant sensing and response forms of the smart drive, stronger response ability, more expansive functional applications were achieved. Therefore, learning from the nature, rationalization of structure, excellent performances, controllability and highly efficient applications of which have been achieved by structural design and integration of ideas. And this biomimic method has become an important direction of nano composites. While we still have many things to do in nano carbon composite materials with this approach and lack a deep understanding of the transformation mechanism between biological structure and function. In this paper, we have reviewed the preparation and processing of high content nano carbon composites and their bionic design of structure and interface. Also the progress in applications of bionic smart drive was introduced. In the end, we discussed the development direction of multifunctional nano carbon composites.