Copper (Cu) is used as an interconnection material in semiconductor industries for years owing to its best balance of conductivity and performance. However, it is running out of steam as it is approaching its limits with respect to electrical performance and reliability. Graphene is a non-metal material, but it can help to improve electromigration (EM) performance of Cu owing to its excellent properties. Combining graphene with copper for VLSI interconnects can be a viable solution. The incorporation of graphene into Cu allows the present Cu fabrication back-end process to remain unaltered, except the small step of inserting graphene into Cu. Therefore, it has a great potential to revolutionize the VLSI-IC industry and appeal for further advancement of semiconductor industry. This book is a compilation of comprehensive studies done on the properties of graphene and its synthesis methods suitable for VLSI interconnects' applications. It includes the development of a new method to synthesize graphene, the evaluation of electrical and EM performance of graphenated Cu interconnects, and a new graphene-based electroless deposition method for Cu and other metals.