The use of oligonucleobase moieties in materials science has experienced growing interest in recent years. Several researchers have elegantly shown the application of oligonucleotides as versatile building blocks for the synthesis of, for example, controlled nanoscaled structures and molecular machines. Also, in polymer science, oligonucleobases have become a topic of investigation. Nucleobase-functionalized polymers have been applied in various applications such as template polymerizations and supramolecular materials, in which the noncovalent anchors are based on oligonucleotides. Lutz et al. found that the incorporation of a complementary nucleobase functionality into synthetic copolymers leads to materials that can exhibit a DNAlike melting behavior. In addition, Rowan and coworkers prepared thermoresponsive supramolecular polymer materials, in which the noncovalent interactions are based on single nucleobase moieties. Recent advances in controlled (radical) polymerization techniques such as atom transfer radical polymerization (ATRP) have further increased activity in the polymer chemistry field. These methods allow the formation of well-defined polymer architectures in which a large variety of biological functionalities, such as nucleobases, can be included. It is well known that amphiphilic block copolymers have the ability to assemble into multiple morphologies in solution. Depending on a number of parameters, such as the ratio of the hydrophilic and hydrophobic blocks, the morphology can vary from spherical micelles, rods, and vesicles to large compound micelles (LCMs). Even more structural control is possible when block copolymers are used that are built up out of a synthetic part and a biomolecular part. Another method was developed by Rotello and coworkers, who prepared plug and play polymers that facilitated recognition through hydrogen-bonding interactions to change the morphology of the polymers or even direct self-assembly of patterned surfaces. Several examples in which peptide sequences are incorporated into polymer chains have been shown to control the material properties and enable self-assembly into well-defined nanoscale architectures. Besides proteins, this could also apply to nucleobase block copolymers. In previous investigations, it already has been demonstrated that the incorporation of small oligonucleotide strands has vast potential to influence the aggregation of block copolymers. Often the incorporation of these biofunctional moieties into the polymer chain facilitates some form of aggregation. Either the aggregation of the biological functionality is enhanced by the polymer chain or aggregation of the polymer chains is increased via specific interactions between the biological functionalities. In addition, the nanocompartmentalization by block copolyCorrespondence to: J. C. M. van Hest (E-mail: j.vanhest@ science.ru.nl)