The construction of well-defined hybrid materials consisting of synthetic polymers and (poly)peptides or proteins has attracted much attention in recent years. Different techniques have become available that allow an efficient synthesis of polymer architectures with (poly)peptides in the side chain as well as the main chain. Oligopeptides modified with monomer or initiator moieties can, for example, be introduced in polymers via controlled (radical) polymerization methods. Ligation methods enable the build up of large peptide structures via a complete organic chemistry approach. The materials scientist's toolbox is enriched with molecular biology techniques, and protein engineering has become a standard synthetic method for the construction of well-defined polypeptides with specific functional handles for the attachment of synthetic polymers. The availability of all these techniques holds much promise for the application of materials in the biomedical field, and especially tissue engineering, targeted drug delivery and diagnostics should in the near future benefit from these recent synthetic achievements.