Understanding the deformation mechanisms of nanocrystalline (nc) metals at the atomic-scale is crucial for determining how far the strengths of metals can be ultimately reached. Although several breakthroughs have been achieved by designing nc metals with ultra-high strength and high ductility [1], the atomistic deformation mechanisms of nc metals with grain sizes of <15 nm have not been fully understood because of the lack of direct atomic-scale experimental evidence [1,2]. For a long time, our understanding of the atomistic deformation mechanisms of nc metals relied heavily on molecular dynamic simulations, which had been the only method for revealing atomic-scale dynamic plastic deformation processes of nc materials [2] before Han and his colleagues developed an experimental technique that allows direct atomic resolution imaging of dynamic tensile deformation processes of nc materials [3,4]. Using this technique, they discovered that the critical size for deformation mode transformation from intra-grain dislocation activities to inter-grain plasticity can be as small as~6 nm, which is far below~15 nmpredicted by MD simulations [1,2]. The discovery set up a milestone for the strength limit of polycrystalline materials since the inverse HallPetch deformation mode was proposed about three decades ago, which indicated the strength of polycrystalline materials could continue to increase by decreasing grain size down to~6 nm. This provides the direct atomic-scale experimental evidence for the upper limit strength of nc metals and important guidance for developing bulk structural materials with ultra-high strength yet with high ductility.With the capability of atomic-scale in situ investigation of the deformation mechanisms of nc metals, a long-time puzzle in nc metals, the deformation twinning nucleation process in high stacking fault energy metals is revealed unambiguously [5]. It has been believed that a deformation twin nucleates through the layer-by-layer slip of partial dislocations on consecutive close-packed atomic planes and that deformation twins should be suppressed in many face-centered cubic (FCC) metals with high unstable twin-fault energy, such as Al, Pt and Pd, in which the formation of twin embryos is difficult [6]. However, this is at odds with extensive experimental observations of deformation twins in these FCC nc metals [7][8][9]. Recently, Han and his colleagues presented atomicresolution in situ evidence of a new route of deformation twinning in nc Pt having a high twin-fault energy [5]. An atomic-scale twinning process was captured in situ in a Cs-corrected transmission electron microscope (TEM).