Low-density materials with tailorable properties have attracted attention for decades, yet stiff materials that can resiliently tolerate extreme forces and deformation while being manufactured at large scales have remained a rare find. Designs inspired by nature, such as hierarchical composites and atomic lattice-mimicking architectures, have achieved optimal combinations of mechanical properties but suffer from limited mechanical tunability, limited long-term stability, and low-throughput volumes that stem from limitations in additive manufacturing techniques. Based on natural self-assembly of polymeric emulsions via spinodal decomposition, here we demonstrate a concept for the scalable fabrication of nonperiodic, shell-based ceramic materials with ultralow densities, possessing features on the order of tens of nanometers and sample volumes on the order of cubic centimeters. Guided by simulations of separation processes, we numerically show that the curvature of self-assembled shells can produce close to optimal stiffness scaling with density, and we experimentally demonstrate that a carefully chosen combination of topology, geometry, and base material results in superior mechanical resilience in the architected product. Our approach provides a pathway to harnessing self-assembly methods in the design and scalable fabrication of beyond-periodic and nonbeam-based nano-architected materials with simultaneous directional tunability, high stiffness, and unsurpassed recoverability with marginal deterioration
