We review the development of ultrafast electron nanocrystallography as a method for investigating structural dynamics for nanoscale materials and interfaces. Its sensitivity and resolution are demonstrated in the studies of surface melting of gold nanocrystals, nonequilibrium transformation of graphite into reversible diamond-like intermediates, and molecular scale charge dynamics, showing a versatility for not only determining the structures, but also the charge and energy redistribution at interfaces. A quantitative scheme for 3D retrieval of atomic structures is demonstrated with few-particle (<1,000) sensitivity, establishing this nanocrystallographic method as a tool for directly visualizing dynamics within isolated nanomaterials with atomic scale spatio-temporal resolution.