In recent years, there has been significant interest in the utilization of natural materials for nanomaterials which impact a broad range of fields including tissue engineering, smart textiles, electronics, energy, coatings and more. Natural polymers such as silk, have received renewed interest due to their unique properties and potential applications. Silk fibers are traditionally 10-20 µm in diameter. This book researches the scientific implications of reducing the diameter to the nanoscale and adding nanofillers in the form of carbon nanotubes by the electrospinning process. The effects of post processing treatments on the physico-chemical properties of the nanofibers were also studied. Statistical analysis was applied to develop processing windows that can reproduce nanofibers less than 100 nm in diameter. The extensive experimental works outlined in this book are creative and commercially justifiable solutions to technical challenges relating to the development, fabrication, characterization, and optimization of next-generation advanced nanomaterials.