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Biological materials such as seashell nacre exhibit extreme mechanical properties due to their multilayered microstructures. Collaborative interaction among these layers achieves performance beyond the capacity of a single layer. Inspired by these multilayer biological systems, we architect materials with free-form layered microstructures to program multistage snap-buckling and plateau responses—accomplishments challenging with single-layer materials. The developed inverse design paradigm simultaneously optimizes local microstructures within layers and their interconnections, enabling intricate layer interactions. Each layer plays a synergistic role in collectively achieving high-precision control over the desired extreme nonlinear responses. Through high-fidelity simulations, hybrid fabrication, and tailored experiments, we demonstrate complex responses fundamental to various functionalities, including energy dissipation and wearable devices. We orchestrate multisnapping phenomena from complex interactions between heterogeneous local architectures to encode and store information within architected materials, unlocking data encryption possibilities. These layered architected materials offer transformative advancements across diverse fields, including vibration control, wearables, and information encryption. 

Abstract Fourier’s law dictates that heat flows from warm to cold. Nevertheless, devices can be tailored to cloak obstacles or even reverse the heat flow. Mathematical transformation yields closed-form equations for graded, highly anisotropic thermal metamaterial distributions needed for obtaining such functionalities. For simple geometries, devices can be realized by regular conductor distributions; however, for complex geometries, physical realizations have so far been challenging, and sub-optimal solutions have been obtained by expensive numerical approaches. Here we suggest a straightforward and highly efficient analytical de-homogenization approach that uses optimal multi-rank laminates to provide closed-form solutions for any imaginable thermal manipulation device. We create thermal cloaks, rotators, and concentrators in complex domains with close-to-optimal performance and esthetic elegance. The devices are fabricated using metal 3D printing, and their omnidirectional thermal functionalities are investigated numerically and validated experimentally. The analytical approach enables next-generation free-form thermal meta-devices with efficient synthesis, near-optimal performance, and concise patterns. 

Programming structures to realize any prescribed mechanical response under large deformation is highly desired for various functionalities, such as actuation and energy trapping. Yet, the use of a single material phase and heuristically developed structural patterns leads to restricted design space and potential failure to achieve specific target behaviors. Here, through a free-form inverse design approach, multiple hyperelastic materials with distinct properties are optimally synthesized into composite structures to precisely achieve arbitrary and extreme prescribed responses under large deformations. The digitally synthesized structures exhibit organic shapes and motions with irregular distributions of material phases. Within the structures, different materials play distinct roles yet seamlessly collaborate through sophisticated deformation mechanisms to produce the target behaviors, some of which are unachievable by a single material. While complex in geometry and material heterogeneity, the discovered structures are effectively manufactured via multimaterial fabrication with different polydimethylsiloxane (PDMS) elastomers with distinct behaviors and their highly nonlinear responses are physically and accurately realized in experiments. To enhance programmability, the synthesized structures are heteroassembled into architectures that exhibit highly complex yet navigable responses. The proposed synthesis, multimaterial fabrication, and heteroassembly strategy can be utilized to design function-oriented and situation-specific mechanical devices for a wide range of applications.