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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. 

Anisotropy in additive manufacturing (AM), particularly in the material extrusion process, plays a crucial role in determining the actual structural performance, including the stiffness and strength of the printed parts. Unless accounted for, anisotropy can compromise the objective performance of topology-optimized structures and allow premature failures for stress-sensitive design domains. This study harnesses process-induced anisotropy in material extrusion-based 3D printing to design and fabricate stiff, strong, and lightweight structures using a two-step framework. First, an AM-oriented anisotropic strength-based topology optimization formulation optimizes the structural geometry and infill orientations, while assuming both anisotropic (i.e., transversely isotropic) and isotropic infill types as candidate material phases. The dissimilar stiffness and strength interpolation schemes in the formulation allow for the optimized allocation of anisotropic and isotropic material phases in the design domain while satisfying their respective Tsai–Wu and von Mises stress constraints. Second, a suitable fabrication methodology realizes anisotropic and isotropic material phases with appropriate infill density, controlled print path (i.e., infill directions), and strong interfaces of dissimilar material phases. Experimental investigations show up to 37% improved stiffness and 100% improved strength per mass for the optimized and fabricated structures. The anisotropic strength-based optimization improves load-carrying capacity by simultaneous infill alignment along the stress paths and topological adaptation in response to high stress concentration. The adopted interface fabrication methodology strengthens comparatively weaker anisotropic joints with minimal additional material usage and multi-axial infill patterns. Furthermore, numerically predicted failure locations agree with experimental observations. The demonstrated framework is general and can potentially be adopted for other additive manufacturing processes that exhibit anisotropy, such as fiber composites.