Molecular dynamics simulations are frequently used to study deformation mechanisms at the nanoscale. However, the lattice orientations of grains in the starting nanocrystalline (nc) configurations are typically based on either random orientations (Van Swygenhoven and Derlet [1]; Schiotz et al. [2]) or orientations specifically chosen to be high angle grain boundaries (Yamakov et al. [3]), which may not be either global or local minimum energy configurations. Our hypothesis is that global or local minimum energy configurations are more representative of actual nc grain structures.