Natural materials, such as bone and abalone nacre, exhibit exceptional mechanical properties, a product of their intricate microstructural organization. Freeze casting is a relatively simple, inexpensive, and adaptable materials processing method to form porous ceramic scaffolds with controllable microstructural features. After infiltration of a second polymeric phase, hybrid ceramic-polymer composites can be fabricated that closely resemble the architecture and mechanical performance of natural bone and nacre. Inspired by the narwhal tusk, magnetic fields applied during freeze casting can be used to further control architectural alignment, resulting in freeze-cast materials with enhanced mechanical properties.