Proteins possess an impressive array of functionality ranging from catalytic activity to selective binding and mechanical strength, making them highly attractive for materials engineering. Conjugation of synthetic polymers to proteins has the potential to improve the physical properties of the protein as well as provide functionality not typically found in native proteins, such as stimuli-responsive behavior and the programmable ability to self-assemble. This viewpoint discusses the design of protein-polymer conjugates, an important class of block copolymers. Use of these hybrid molecules in biological and catalytic applications is highlighted, and the ability of the polymer to direct the solution and solid-state self-assembly of the hybrid block copolymers is reviewed. Future challenges in polymer and material science that will enable these hybrid molecules to reach their potential as protein-based materials are outlined.