AbstractNature is very successful in designing strong and tough, lightweight materials. Examples include seashells, bone, teeth, fish scales, wood, bamboo, silk, and many others. A distinctive feature of all these materials is that their properties are far superior to those of their constituent phases. Many of these natural materials are lamellar or layered in nature. With its “brick and mortar” structure, nacre is an example of a layered material that exhibits extraordinary physical properties. Finding inspiration in living organisms to create bioinspired materials is the subject of intensive research. Several processing techniques have been proposed to design materials mimicking natural materials, such as layer‐by‐layer deposition, self‐assembly, electrophoretic deposition, hydrogel casting, doctor blading, and many others. Freeze casting, also known as ice‐templating, is a technique that has received considerable attention in recent years to produce bioinspired bulk materials. Here, recent advances in the freeze‐casting technique are reviewed for fabricating lamellar scaffolds by assembling different dimensional building blocks, including nanoparticles, polymer chains, nanofibers, and nanosheets. These lamellar scaffolds are often infiltrated by a second phase, typically a soft polymer matrix, a hard ceramic matrix, or a metal matrix. The unique architecture of the resultant bioinspired structural materials displays excellent mechanical properties. The challenges of the current research in using the freeze‐casting technique to create materials large enough to be useful are also discussed, and the technique's promise for fabricating high‐performance nacre‐inspired structural materials in the future is reviewed.