The conjugation of biomacromolecules, such as proteins, to polymeric materials has many applications. These applications are as varied as the formation of protein−polymer conjugates used in therapeutic treatments to applications in sensors, biocatalysts, and tools for separation of biomolecules. The diverse range of hybrid materials available necessitates a diverse range of corresponding methodologies to support their construction. Among the key focuses of this thesis includes methodologies for the development of protein−polymer biomaterials and their wide-ranging applications. The first chapter is a review of methods of site-selective protein conjugation with polymers via naturally encoded sequences. This review covers a variety of methodologies for protein−polymer conjugation moving from non-specific methods to more sophisticated, site-selective methods. The second chapter will review the structure and applications of protein-biomaterials, such as those conjugated to a nano-object or immobilized to a solid substrate. The second chapter will also cover the enhanced properties of novel materials at the interphase between nano, surface, and biological chemistry. The development of a boronic acid resin for the selective immobilization of canonically encoded (pyroglutamate-histidine-tagged) proteins is covered in the third chapter. The fourth chapter demonstrates a unique application of these protein−polymer biomaterials as a template in the synthesis of fluorescent copper nanoclusters. The fifth chapter will focus on efforts towards the controlled release of boronic acid-based therapeutics by tailoring boronate ester hydrolysis kinetics. Finally, the sixth chapter will showcase the antibacterial activity of capacitively coupled plasma from laser-induced graphene and the experiments elucidating the molecular mediator of bacterial cell death.