Smaller is stronger," sub-, micro-, and nanomaterials exhibit high strength, ultralarge elasticity and unusual plastic and fracture behaviors which originate from their size effect and the low density of defects, different from their conventional bulk counterparts. To understand the structural evolution process under external stress at atomic scale is crucial for us to reveal the essence of these "unusual" phenomena and is momentous in the design of new materials. Our review presents the recent developments in the methods, techniques, instrumentation, and scientific progress of atomic scale in situ deformation dynamics on single crystalline nanowires. The super-large elasticity, plastic deformation mechanism transmission, and unusual fracture behavior related to the experimental mechanics of nanomaterials are reviewed. In situ experimental mechanics at the atomic scale open a new research field which is important not only to the microscopic methodology but also to the practice.