Deformation twinning in pure aluminum has been considered to be a unique property of nanostructured aluminum. A lingering mystery is whether deformation twinning occurs in coarse-grained or single-crystal aluminum, at scales beyond nanotwins. Here, we present the first experimental demonstration of macro deformation twins in single-crystal aluminum formed under ultrahigh strain-rate (∼10 6 s −1 ), large shear strain (200%) via dynamic equal channel angular pressing. Deformation twinning is rooted in the rate dependences of dislocation motion and twinning, which are coupled, complementary processes during severe plastic deformation under ultrahigh strain rates.When we talk about crystal deformation, what do we actually talk about? Crystal defects [1]. Crystal defects such as dislocations (line defects) and twins (planar defects) play a critical role in plastic deformation and ultimately govern the multifarious mechanical behaviors of many crystalline materials [2,3]. While both dislocation slip and deformation twinning are dependent on an intrinsic material property -stacking fault energy [4,5] (SFE), their sensitivities to SFE differ considerably. A notable example is pure aluminum, a typical face-centered cubic (fcc) metal with high SFE (104-142 mJ m −2 ) [6], in which deformation twinning rarely occurs even deformed at low temperatures and/or at high strain rates [7,8]. This rareness of deformation twinning in such materials is normally attributed to the following two reasons: (i) a large number of slip systems in fcc metals render dislocation slip a very efficient deformation mode [9,10], and (ii) the nucleation of twinning partial dislocations require much higher shear stresses than trailing partial dislocations due to the high unstable twin fault energy [11]. Searching for macro deformation twins in pure aluminum and revealing the underlying mechanisms have been of sustained interest in the past decade.Molecular dynamics (MD) simulations first predicted that nanoscale deformation twins can nucleate under high tensile stress (2.5 GPa) and high strain rate (10 7 s −1 ) in nanograined aluminum [6,12], and subsequent experiments confirmed this prediction in nanograined aluminum films under different kinds of severe plastic deformation (SPD) [13][14][15]. One explanation was proposed based on classical dislocation theory [16]: when grain size decreases to tens of nanometers, normal dislocation activities are greatly suppressed by the high fraction of grain boundaries (GBs); as a result, deformation twinning takes over as the dominant deformation mechanism [13]. Besides nanograin size effect, many simulation and experimental studies suggest that deformation twinning prefers to occur at high strain rates in fcc metals [17,18]. This rate-dependent twinning mechanism has been corrobarated by a very recent experiment on pure aluminum with comparatively large nanograins (50-100 nm) [19]. However, there has been no solid evidence for deformation twinning in single-crystal or coarse-grained pure aluminum. It is natural ...