Grain boundary (GB) is the interface between different oriented crystals of the same material, and it can have a significant effect on the many properties of materials. When the average or entire range of grain size is reduced to less than 100 nm, the conventional plastic deformation mechanisms dominated by dislocation processes become difficult and GBmediated deformation mechanisms become increasingly important. One of the mechanisms that can play a profound role in the strength and plasticity of metallic polycrystalline materials is the heterogeneous nucleation and emission of dislocations from GB. In this study, we conducted molecular dynamics simulations to study the dislocation nucleation from copper bicrystal with a number of 〈1 10〉 tilt GBs that covered a wide range of misorientation angles (θ).Wewill show from this analysis that the mechanic behavior of GBs and the energy barrier of dislocation nucleation from GBs are closely related to the lattice crystallographic orientation, GBenergy, and the intrinsic GBstructures. An atomistic analysis of the nucleation mechanisms provided details of this nucleation and emission process that can help us to better understand the dislocation source in GB.