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Twin boundary (TB) strengthening in nanotwinned metals experiences a breakdown below a critical spacing at which softening takes over. Here, we survey a range of nanotwinned materials that possess different stacking fault energies (SFEs) and understand the TB strengthening limit using atomistic simulations. Distinct from Cu and Al, the nanotwinned, ultralow SFE materials (Co, NiCoCr, and NiCoCrFeMn) intriguingly exhibit a continuous strengthening down to a twin thickness of 0.63 nm. Examining dislocation slip mode and deformation microstructure, we find the hard dislocation modes persist even when reducing the twin boundary spacing to a nanometer regime. Meanwhile, the soft dislocation mode, which causes detwinning in Cu and Al, results in phase transformation and lamellar structure formation in Co, NiCoCr, and NiCoCrFeMn. This study, providing an enhanced understanding of dislocation mechanism in nanotwinned materials, demonstrates the potential for controlling mechanical behavior and ultimate strength with broadly tunable composition and SFE, especially in multi-principal element alloys.

Failure of materials and structures is inherently linked to localized mechanisms, from shear banding in metals, to crack propagation in ceramics and collapse of space‐trusses after buckling of individual struts. In lightweight structures, localized deformation causes catastrophic failure, limiting their application to small strain regimes. To ensure robustness under real‐world nonlinear loading scenarios, overdesigned linear‐elastic constructions are adopted. Here, the concept of delocalized deformation as a pathway to failure‐resistant structures and materials is introduced. Space‐tileable tensegrity metamaterials achieving delocalized deformation via the discontinuity of their compression members are presented. Unprecedented failure resistance is shown, with up to 25‐fold enhancement in deformability and orders of magnitude increased energy absorption capability without failure over same‐strength state‐of‐the‐art lattice architectures. This study provides important groundwork for design of superior engineering systems, from reusable impact protection systems to adaptive load‐bearing structures.