A multiscale and multi-physical model which could couple dislocation dynamics and finite element method was developed to simulate the mechanical response of nanostructural metals. The multiscale model can capture detailed dynamics evolution of dislocation structures and can predict macroscopic constitutive response. In addition, the developed model could account for complex multi-physical phenomena, which would play an important role in obtaining a fundamental understanding of deformation mechanism in nanostructural metals. Applications of developed concurrent coupled model includes Taylor impact test, nanoindentation, and hydrogen embrittlement at submicron length scale. The developed model will shed light on fundamental investigation of “defect-controlled” mechanical behaviors in nanostructural metals.