Inspired by the controversy over tensile deformation modes of single-crystalline 〈110〉/{111} Au nanowires, we investigated the dependency of the deformation mode on diameters of nanowires using the molecular dynamics technique. A new criterion for assessing the preferred deformation mode—slip or twin propagation—of nanowires as a function of nanowire diameter is presented. The results demonstrate the size-dependent transition, from superplastic deformation mediated by twin propagation to the rupture by localized slips in deformed region as the nanowire diameter decreases. Moreover, the criterion was successfully applied to explain the superplastic deformation of Cu nanowires.