AbstractNanotwinned materials have been widely studied as a promising class of nanostructured materials that exhibit an exceptional combination of high strength, good ductility, large fracture toughness, remarkable fatigue resistance, and creep stability. Recently, an apparent controversy has emerged with respect to how the strength of nanotwinned materials varies as the twin thickness is reduced. While a transition from hardening to softening was observed in nanotwinned Cu when the twin thickness is reduced below a critical value, continuous hardening was reported in nanotwinned ceramics and nanotwinned diamond. Here, by conducting atomistic simulations and developing a theoretical modeling of nanotwinned Pd and Cu systems, we discovered that there exists a softening temperature, below which the material hardens continuously as the twin thickness is reduced (as in nanotwinned ceramics and diamond), while above which the strength first increases and then decreases, exhibiting a maximum strength and a hardening to softening transition at a critical twin thickness (as in nanotwinned Cu). This important phenomenon has been attributed to a transition from source- to stress-controlled plasticity below the softening temperature, and suggests that different hardening behaviors may exist even in the same nanotwinned material depending on the temperature and that at a given temperature, different materials could exhibit different hardening behaviors depending on their softening temperature.