The combination of nanotechnology with green chemistry has become a major factor to determine the future of nanotechnology. The use of natural products for the synthesis of nanomaterials, especially the green growth of carbon-based nanomaterials has extensively been explored and many of these products are now finding their way from the laboratory to various fields of engineering and technology. Nanostructures of carbon include tubes, spherical, or single-layered with fundamentally different properties. These carbon nanostructures have numerous technological applications in microelectronics and nanoelectronics, displays, durable batteries, biosensors, etc. However, the applications of these carbon-based nanomaterials still face significant challenges. This chapter presents the development of green carbon-based nanostructures, recent advances, and the challenges and applications of these nanomaterials.