In present chapter, the evolution of carbon-based nanomaterials (CNMs) is elaborately discussed. The structure performance relationship based upon the unique properties of CNMs is established. The synthesis of CNMs is briefly predicted with schematic representation. The preliminary idea regarding nanohorns, nanodiamonds, and nano-onions is presented in the chapter whose applications in detail are extensively investigated in different chapters of this book. This chapter is concluded with predicting various applications of CNMs. Out of different applications, CNMs as drug delivery vehicles are the main motivation of this book.