Nanotwins require little energy to form in metals, but their impact on strength and ductility is dramatic. New mechanisms of strengthening, strain hardening, ductility, and strain-rate sensitivity have been observed in nanowires, films, and bulk materials containing nanoscale twins as the twin-boundary spacing decreases. These mechanisms can act in concert to produce interface-dominated nanomaterials with extreme tensile strength and plastic deformation without breaking. This article reviews recent theoretical and experimental understanding of the physical mechanisms of plasticity in nanotwin-strengthened metals, with a particular focus on the fundamental roles of coherent, incoherent, and defective twin boundaries in plastic deformation of bulk and small-scale cubic systems, and discusses new experimental methods for controlling these deformation mechanisms in nanotwinned metals and alloys.