“…Therefore, optimizing the sequence of monomers in the block copolymer chain can not only alter the dynamics of the chains, chain conformations, and morphologies but also enable the design of materials with predictable properties. − Consequently, the identification of an optimum balance between the hydrophobic and hydrophilic segments within the polymers is determined by packing parameters, ultimately leading to the formation of specific self-assembled nanostructures. − Notably, stimuli-responsive chain collapse could induce a change in the packing parameter, potentially resulting in a transformation of the self-assembled nanostructures. , Armes et al demonstrated such stimuli-responsive chain collapse in the poly( N -(2-acryloyloxyethyl)pyrrolidone)–poly(4-hydroxybutyl acrylate) (PNAEP 85 –PHBA x ) diblock copolymer by increasing the pH of the dispersion above the p K a of terminal carboxylic acid, leading to the chain-induced vesicle-to-sphere transition . In another report, Harrison et al reported reversible morphological transformations from spheres to worms and vesicles dictated by the pH of the surrounding medium in a pH-responsive copolymer composed of acrylic acid and butyl acrylate. , In that regard, our group demonstrated an interesting stimuli-responsive chain collapse strategy to alter polymeric nanostructures for application in photoresponsive self-healable coating and drug delivery applications. − Further, we have also exploited such stimuli-responsive polymer chain folding to design interesting peptide–polymer conjugate networks with exciting nonlinear mechanical properties and piezoelectric behavior. − Recently, we have demonstrated that an amphiphilic diblock polymer with stimuli-responsive moieties in the hydrophobic domain can exhibit chain collapse behavior in response to external stimuli, leading to reversible transformation of vesicles to micelles by fine-tuning the packing parameter . Thus, the coassembled vesicles, influenced by orthogonal stimuli, formed self-sorted compartments, offering potential applications in mimicking interactions of artificial cell models with the extracellular matrix.…”