Nature is unparalleled in its structural and functional diversity. Living organisms make fantastic materials under myriad conditions with properties we cannot emulate today using conventional approaches. In many cases, nature has provided us with a blueprint to design and assemble both natural and synthetic building blocks to create a new generation of functional, organized, and responsive materials. We have taken cues from nature to design materials with unique structural and functional properties, along with new process technologies with the ability to produce a wide range of biomimetic structures. Specifically, we have focused on the generation of nanostructures that are functionalized with and in some cases constructed from biological molecules, complete with tailored selectivities and biocatalytic activities. For example, these nanostructures have been exploited in the generation of biocatalytically functional polymeric films, coatings, and paints.