This chapter reviews the Chemical Vapor Deposition (CVD) technologies for polycrystalline silicon (Si), metals and insulator which were developed for application to Mbit-scale device processes and research efforts for Gbit-scale ultra large scale integrated circuits (ULSI) processes. It presents thermal CVD and plasma CVD of the insulators for multilayer interconnection developed for Mbit scale VLSI. The chapter also presents the CVD of new materials such as low dielectric constant and high dielectric constant insulators which are developing for Gbitscale ULSI devices. CVD of various materials has been studied with a view to application in VLSI fabrication. Polycrystalline Si has been used widely in VLSI devices, for example, for the gate and capacitor electrode, for diffusion sources, and for interconnection wire. Many applications of polycrystalline Si require controllable doping to reduce resistivity. Some techniques to improve step coverage of reactive sputtering have been studied, such as collimated sputtering and long through sputtering.