Protein-based polymeric materials are characterized by multi-functionality, complex structural diversity, and bioactivity. Using protein-based biomaterials may substantially increase the efficacy of regenerative medicine therapies by providing cell-protein interactions that guide cell behavior. Several examples of protein-based biomaterials design will be presented to highlight the importance of independent control over biochemical and biomechanical properties. Using recombinant protein technology, we have synthesized several families of block-co-peptide hydrogels that mimic critical aspects of the natural extracellular matrix. A modular design strategy enables independent tuning of the initial elastic modulus, the density of cell adhesion ligands, and the rate of proteolytic remodeling. These biomaterials can be designed to release multiple therapeutic peptides with distinct spatial and temporal delivery profiles. Protein-based materials can also be used as templates to guide the synthesis of inorganic nanomaterials. Specifically, we are utilizing the protein clathrin, which has the ability to form multiple 2D and 3D architectures, as a flexible template that can be functionalized at specific sites using designed bi-functional peptides. These peptides serve as molecular bridges between binding sites on the clathrin protein and inorganic materials including gold, titania, and cobalt oxide. By generating a family of engineered peptides, we are developing a flexible, modular system that will enable the rapid development of multiple inorganic nanostructures from a single protein template material.