Four-dimensional (4D) printing involves conventional 3D printing followed by a shape-morphing step. It enables more complex shapes to be created than is possible with conventional 3D printing. However, 3D-printed ceramic precursors are usually difficult to be deformed, hindering the development of 4D printing for ceramics. To overcome this limitation, we developed elastomeric poly(dimethylsiloxane) matrix nanocomposites (NCs) that can be printed, deformed, and then transformed into silicon oxycarbide matrix NCs, making the growth of complex ceramic origami and 4D-printed ceramic structures possible. In addition, the printed ceramic precursors are soft and can be stretched beyond three times their initial length. Hierarchical elastomer-derived ceramics (EDCs) could be achieved with programmable architectures spanning three orders of magnitude, from 200 μm to 10 cm. A compressive strength of 547 MPa is achieved on the microlattice at 1.6 g cm⁻³. This work starts a new chapter of printing high-resolution complex and mechanically robust ceramics, and this origami and 4D printing of ceramics is cost-efficient in terms of time due to geometrical flexibility of precursors. With the versatile shape-morphing capability of elastomers, this work on origami and 4D printing of EDCs could lead to structural applications of autonomous morphing structures, aerospace propulsion components, space exploration, electronic devices, and high-temperature microelectromechanical systems.

Wear-related energy and material loss cost over 2500 Billion Euro per year. Traditional wisdom suggests that high-strength materials reveal low wear rates, yet, their plastic deformation mechanisms also influence their wear performance. High strength and homogeneous deformation behavior, which allow accommodating plastic strain without cracking or localized brittle fracture, are crucial for developing wear-resistant metals. Here, we present an approach to achieve superior wear resistance via in-situ formation of a strong and deformable oxide nanocomposite surface during wear, by reaction of the metal surface with its oxidative environment, a principle that we refer to as ‘reactive wear protection’. We design a TiNbZr-Ag alloy that forms an amorphous-crystalline oxidic nanocomposite surface layer upon dry sliding. The strong (2.4 GPa yield strength) and deformable (homogeneous deformation to 20% strain) nanocomposite surface reduces the wear rate of the TiNbZr-Ag alloy by an order of magnitude. The reactive wear protection strategy offers a pathway for designing ultra-wear resistant alloys, where otherwise brittle oxides are turned to be strong and deformable for improving wear resistance.

High strength and high ductility are often mutually exclusive properties for structural metallic materials. This is particularly important for aluminum (Al)-based alloys which are widely commercially employed. Here, we introduce a hierarchical nanostructured Al alloy with a structure of Al nanograins surrounded by nano-sized metallic glass (MG) shells. It achieves an ultrahigh yield strength of 1.2 GPa in tension (1.7 GPa in compression) along with 15% plasticity in tension (over 70% in compression). The nano-sized MG phase facilitates such ultrahigh strength by impeding dislocation gliding from one nanograin to another, while continuous generation-movement-annihilation of dislocations in the Al nanograins and the flow behavior of the nano-sized MG phase result in increased plasticity. This plastic deformation mechanism is also an efficient way to decrease grain size to sub-10 nm size for low melting temperature metals like Al, making this structural design one solution to the strength-plasticity trade-off.

High‐entropy alloys (HEAs) and metallic glasses (MGs) are two material classes based on the massive mixing of multiple‐principal elements. HEAs are single or multiphase crystalline solid solutions with high ductility. MGs with amorphous structure have superior strength but usually poor ductility. Here, the stacking fault energy in the high‐entropy nanotwinned crystalline phase and the glass‐forming‐ability in the MG phase of the same material are controlled, realizing a novel nanocomposite with near theoretical yield strength (G/24, where G is the shear modulus of a material) and homogeneous plastic strain above 45% in compression. The mutually compatible flow behavior of the MG phase and the dislocation flux in the crystals enable homogeneous plastic co‐deformation of the two regions. This crystal–glass high‐entropy nanocomposite design concept provides a new approach to developing advanced materials with an outstanding combination of strength and ductility.

Interstitials, e.g., C, N, and O, are attractive alloying elements as small atoms on interstitial sites create strong lattice distortions and hence substantially strengthen metals. However, brittle ceramics such as oxides and carbides usually form, instead of solid solutions, when the interstitial content exceeds a critical yet low value (e.g., 2 at.%). Here we introduce a class of massive interstitial solid solution (MISS) alloys by using a highly distorted substitutional host lattice, which enables solution of massive amounts of interstitials as an additional principal element class, without forming ceramic phases. For a TiNbZr-O-C-N MISS model system, the content of interstitial O reaches 12 at.%, with no oxides formed. The alloy reveals an ultrahigh compressive yield strength of 4.2 GPa, approaching the theoretical limit, and large deformability (65% strain) at ambient temperature, without localized shear deformation. The MISS concept thus offers a new avenue in the development of metallic materials with excellent mechanical properties.