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Abstract

Polymersomes exhibit increased stability and reduced permeability compared to conventional lipid‐based compartments—making them an increasingly popular choice for the bottom‐up construction of synthetic cells. Here, the contraction and expansion of functionalized polymersome networks controlled by cholesterol‐tagged deoxyribonucleic acid (DNA) is demonstrated. Different types of block‐copolymer membranes are systematically screened to design a general framework for the self‐assembly of cholesterol‐tagged DNA into the polymersome membrane. Since the developed approach is DNA‐based, the individual symmetric and asymmetric functionalization of the inner and outer polymersome leaflets is possible, a feature which makes it unique in terms of anchoring flexibility and efficiency. In addition to the variety with regard to functionalization, the choice of DNA and temperature can also be used to manipulate the polymersome contact line and the polymersome bending energy. Overall, the strategy potentially allows for the unprecedented possibility to precisely control the contraction and expansion of polymersome network assembly.