Cuttlebone, the endoskeleton of cuttlefish, offers an intriguing biological structural model for designing low-density cellular ceramics with high stiffness and damage tolerance. Cuttlebone is highly porous (porosity ~93%) and lightweight (density less than 20% of seawater), constructed mainly by brittle aragonite (95 wt%), but capable of sustaining hydrostatic water pressures over 20 atmospheres and exhibits energy dissipation capability under compression comparable to many metallic foams (~4.4 kJ/kg). Here we computationally investigate how such a remarkable mechanical efficiency is enabled by the multiscale structure of cuttlebone. Using the common cuttlefish, Sepia Officinalis, as a model system, we first conducted high-resolution synchrotron micro-computed tomography (µ-CT) and quantified the cuttlebone's multiscale geometry, including the 3D asymmetric shape of individual walls, the wall assembly patterns, and the long-range structural gradient of walls across the entire cuttlebone (ca. 40 chambers). The acquired 3D structural information enables systematic finite-element simulations, which further reveal the multiscale mechanical design of cuttlebone: at the wall level, wall asymmetry provides optimized energy dissipation while maintaining high structural stiffness; at the chamber level, variation of walls (number, pattern, and waviness amplitude) contributes to progressive damage; at the entire skeletal level, the gradient of chamber heights tailors the local mechanical anisotropy of the cuttlebone for reduced stress concentration. Our results provide integrated insights into understanding the cuttlebone's multiscale mechanical design and provide useful knowledge for the designs of lightweight cellular ceramics. Upon the prior curvature analysis of the cuttlebone walls, we discovered that the walls were primarily "saddle-shaped". Thus, the characterization of different curvatures, varying between flat, domed, saddled, or cylindrical surfaces, were explored. A mathematical model was utilized to generate multiple walls with different curvature characteristics. We observed the mechanical performance of these walls via finite-element analysis and formulated different techniques for designing effective ceramic structures through incorporation of curvature. / Master of Science / The cuttlefish is a marine species that instead of having an inflatable swim bladder like fish, is a mollusk capable of swimming by utilizing their skeleton, called the cuttlebone. The cuttlefish can freely traverse the waters by controlling the flow of water in and out of their brittle skeletons, changing their buoyancy. For this reason, the cuttlebone must be very porous yet strong to withstand the deep-water pressures, enticing an interest for closer observation of the structure which may be useful in engineering applications involving ceramic structures. In this study, we examined an actual cuttlebone structure to better visualize its features with high-resolution synchrotron micro-computed tomography (µ-CT) and tabulated its mechanical performance through a variety of tests using computational software. The skeletal design of the cuttlebone consists of multiple layered chambers supported by wavy, pillar-like walls. It was revealed that the cuttlebone is remarkable due to its multiscale design: the asymmetric geometry of the walls are designed to tolerate considerable amounts of energy while a stiff construction; at the chamber level, variation of walls (number, pattern, and waviness amplitude) helps avoid complete destruction of the structure in the event of an excessive force; at the entire skeletal level, various of chamber heights reduces inflicted stress in concentrated regions of the cuttlebone. The wavy walls were also observed to retain a saddle-shaped curviness, versus simple flat, domed, or cylindrical shaped walls. This created an incentive to explore the effects of curvature on the structural integrity of brittle ceramic structures. We developed an effective way for generating walls with different curvatures and observed the mechanical performance of each wall by crushing them in computer simulations. It was identified that adding curvature to brittle walls prolonged the failure period significantly. While the cylindrical walls were found to be rather stiff, saddle-shaped walls, although not capable of withstanding as much force as flat or cylindrical walls, has a more progressive failure behavior meanwhile maintaining high energy absorption, hence the saddled walls of the cuttlebone to allow maintenance and self-repair in damaged regions.