One-dimensional (1D) and two-dimensional (2D) nanostructures possess many extraordinary structural and physical/chemical properties, and are pursued for a number of innovative devices and material systems in nano science and engineering, such as nano electronics, sensors and composites. Due to their large surface-to-volume ratios, the interface in these nanostructure-based material systems plays important roles in their functionalities and performance. In this chapter, we review the fundamental knowledge of interfacial interactions and their roles in the structural and physical properties, and applications of 1D and 2D nanostructures, and survey the recent advances on the characterization of interfacial interactions in 1D and 2D nanostructure-based material systems.