Biological materials naturally display an astonishing variety of sophisticated nanostructures that are difficult to obtain even with the most technologically advanced synthetic methodologies. As the needs for nanoengineered materials with improved performance characteristics are becoming increasingly important, the potential of biological scaffolds for the fabrication of novel types of nanostructures is being actively explored. This review presents an overview of “biotemplating” as an emerging, unique approach for the synthesis and organization of inorganic nanostructures into well-defined architectures. The technological significance of these architectures is emphasized. We review examples of biological templates explored to date (in terms of their origin and structure) and the success of a variety of methodologies in providing control over the size, crystallinity, and surface chemistry of the nanomaterials.