Hexagonal close-packed (hcp) metals such as Mg, Ti, and Zr are lightweight and/or durable metals with critical structural applications in the automotive (Mg), aerospace (Ti), and nuclear (Zr) industries. The hcp structure, however, brings significant complications in the mechanisms of plastic deformation, strengthening, and ductility, and these complications pose significant challenges in advancing the science and engineering of these metals. In hcp metals, generalized plasticity requires the activation of slip on pyramidal planes, but the structure, motion, and cross-slip of the associated 〈c + a〉 dislocations are not well established even though they determine ductility and influence strengthening. Here, atomistic simulations in Mg reveal the unusual mechanism of 〈c + a〉 dislocation cross-slip between pyramidal I and II planes, which occurs by cross-slip of the individual partial dislocations. The energy barrier is controlled by a fundamental step/ jog energy and the near-core energy difference between pyramidal 〈c + a〉 dislocations. The near-core energy difference can be changed by nonglide stresses, leading to tension-compression asymmetry and even a switch in absolute stability from one glide plane to the other, both features observed experimentally in Mg, Ti, and their alloys. The unique cross-slip mechanism is governed by common features of the generalized stacking fault energy surfaces of hcp pyramidal planes and is thus expected to be generic to all hcp metals. An analytical model is developed to predict the cross-slip barrier as a function of the near-core energy difference and applied stresses and quantifies the controlling features of cross-slip and pyramidal I/II stability across the family of hcp metals.P lastic deformation of crystalline materials occurs mainly by slip along low-index atomic planes. Slip regions are bounded by line defects called dislocations (1), which are characterized by the crystallographic slip increment known as the Burgers vector b and the local line direction ξ. The transition from slipped to unslipped regions is resolved at the atomic scale by local atomic rearrangements creating a dislocation "core" structure. Slip occurs by motion of this core, and the surrounding elastic fields, driven by an applied stress. Plasticity is thus controlled by the details of the core region, which differ significantly among face-centered cubic (fcc), bodycentered cubic (bcc), and hexagonal close-packed (hcp) metals (2). The motion of the dislocation core is usually confined to glide within the slip plane defined by the normal vector n = b × ξ. Screw dislocations have b × ξ = 0, however, and so do not have a unique slip plane and can therefore "cross-slip" among glide planes that share a common Burgers vector. Cross-slip is a crucial process in plasticity, acting to spread slip spatially on multiple nonparallel planes and to enable dislocation multiplication and annihilation processes; all of these processes affect ductility and ultimate strength of the material. Whereas the atomistic mecha...