<p>Ni-based single-crystal superalloys have been widely utilized in aero-engines and turbine blades due to their exceptional mechanical properties. However, there has been a lack of comprehensive studies on the orientation-dependent deformation behaviors of these superalloys. Here, we investigated the interfacial dislocation structures of γ/γ′ phase interfaces with (100), (110), and (111) orientations and calculated the interfacial energies. The results suggested that the (100) interface is the most stable configuration among these interfaces. Furthermore, we conducted large-scale atomistic simulations to investigate the deformation behaviors of Ni-based single-crystal superalloys under uniaxial tension, focusing on the influence of a single nanovoid and its position on mechanical properties. The simulation results showed that the dissociation of the dislocation network at interfaces or dislocation emission from interfaces are the dominant deformation mechanisms at yielding. Moreover, the results indicated that the presence of a single nanovoid alters the stress distribution and leads to complicated interactions with the dislocation network, affecting the dissociation of the dislocation network and the dislocation emission. These findings shed light on the interfacial structures and plastic deformation behaviors of Ni-based single-crystal superalloys, providing guidance for designing and manufacturing superalloys with superior mechanical properties.</p>