Proteins represent the most versatile building blocks available to living organisms or the laboratory scientist for constructing functional materials and molecular devices as well as biological coordination complexes. Underlying this versatility is an immense structural and chemical heterogeneity that renders the programmable self-assembly of proteins a difficult design task. To circumvent the challenge of designing extensive non-covalent interfaces for controlling protein self-assembly, our group has endeavored to use chemical bonding strategies based on fundamental principles of inorganic chemistry and supramolecular chemistry. These strategies have resulted in discrete or infinite, 0-, 1-, 2- and 3D protein architectures that display high structural order over large length scales, yet are dynamic, adaptive and possess new emergent chemical/physical properties. In this talk, I will present some of these functional protein-based materials constructed in our laboratory.