Interface widely exists in carbon nanotube (CNT) assembly materials, taking place at different length scales. It determines severely the mechanical properties of these assembly materials. In this chapter, I assess the mechanical properties of individual CNTs and CNT bundles, the interlayer or intershell mechanics in multiwalled CNTs, the shear properties between adjacent CNTs, and the assembly-dependent mechanical and multifunctional properties of macroscopic CNT fibers and films.