Well-defined block copolymers, comprising bio-related monomers could be conveniently synthesized via Atom Transfer Radical Polymerization. Elastin side chain triblock copolymers were prepared by macroinitiation from a bifunctional polyethylene glycol initiator. The obtained oligopeptide architecture exhibited similar thermoresponsive behavior as its main chain polymer analog. ATRP was performed on methacrylate functionalized nucleobases using an initiator equipped with a primary amine moiety. The resulting nucleobase polymers were successfully coupled to telechelic isocyanate-functional polymethylacrylate, resulting in triblock copolymers that could be interesting building blocks for supramolecular polymers.