The surprising strength and ductility of nacre (in light of its largely ceramic composition) can be attributed to its unique microstructure, which consists of precisely aligned ceramic platelets (bricks) bonded together with nanoscale organic layer (mortar). The underlying composites concepts are arguably straight-forward: (i) high stiffness is maintained by limiting volume fraction of the compliant phase, (ii) high strength is achieved by utilization of small-volume ceramics and an interlocking brick architecture, and (iii) ductility is promoted by brick pull-out. This talk will describe the opportunities and challenges related to the development of synthetic materials that aim to simultaneously implement these concepts. Micromechanical models and large-scale parallelized simulations will be used to describe the key scaling relationships between constituent properties and geometry that control competing deformation mechanisms and govern macroscopic properties. These scaling relationships will be used to identify microstructrual processing targets for high performance materials. The opportunities and challenges relating to realizing these targets will be briefly described in the context of three-dimensional printing of hierarchical structural materials