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In the past few decades, protein–(bio)polymer conjugates have received increasing interest for various technological applications in biomedical and material sciences. By combining synthetic and bio-polymers, sophisticated hybrid materials that outperform their individual components were devised. Having addressed the merits of the functional aspects in these monomeric molecular biohybrids, attention has shifted to their self-assembly capabilities. This step is necessary to confer a higher order of complexity, such as hierarchical structures and functions, as can be observed in macromolecular complexes adopted in Nature. This chapter seeks to give a broad overview of the molecular interactions employed in the self-assembly strategies and the different classes of protein–(bio)polymer hybrids that have been utilized to accomplish functional architectures, which hold immense potential for biological applications.

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