Nanocrystalline materials have been found to deform by mechanisms not accessible to their coarse-grained counterparts. These deformation mechanisms have rendered nanocrystalline materials unique mechanical behaviors such as high strength, low work hardening rate, high strain rate sensitivity, and usually low ductility In a few cases, both high strength and high ductility were observed simultaneously. To understand the mechanical behaviors of nanocrystalline materials and to design them for desired mechanical properties, it is critical to fully understand their deformation mechanisms. Significant progresses have been reported in the last few years on both the deformation mechanisms and mechanical behaviors of nanocrystalline materials. Here a brief overview on the deformation mechanisms of nanocrystalline materials is presented.