Natural materials display a wealth of structures and fulfill a variety of functions. Hierarchical structuring is one of the keys to providing multifunctionality and to adapting to varying needs of an organism. As a consequence, the natural environment represents not only a direct and renewable source of useful materials, such as wood, plant fibers, or even proteins of pharmaceutical importance, but also an enormous “database” of structures with exceptional mechanical, optical, or magnetic properties. Rather than focusing on the direct use of natural materials, this article discusses the use of structures that appeared in evolution and have been implemented in artificial materials of an entirely different type and chemical composition. This may be done either by directly copying the structure (biotemplating) or by extracting the design principles encoded in them for the fabrication of novel bioinspired materials.