This talk reports fundamental calculations and experimental work for covalent bond formation of vertically-oriented carbon nanotubes (CNTs) and copper metals at low temperature. Our goal is to simulate the intra-molecular electron transport among metal-organic materials and reduce the impedance that develops at their interface. In addition, covalent bonds between Cu atoms and CNTs is highly desired in order to create a robust connection that can anchor nanomaterials onto macroscopic metals. Unlike traditional methods that rely on synthesis (~600 °C), this work bonds CNTs to copper at 120 °C. The reported theoretical calculations demonstrate that C atoms on aminophenyl (linker) can form a bridge like covalent bonds with two adjacent Cu atoms on (100), (110), and linear bond on (111) lattice substrates. The reported covalent bond formation is expected to facilitate the application of CNTs in multiple fields such as biomaterials, electrocatalysis, sensor development and electronics.