Nethmi De Alwis Watuthanthrige, Victoria Lohmann, Viviane Lutz‐Bueno, Nghia P. Truong, Steven P. Armes, Athina Anastasaki
Depolymerization offers a powerful route for the chemical recycling of vinyl polymers. However, current strategies focus almost exclusively on monomer recovery, which overlooks broader applications and opportunities. Herein, depolymerization-induced morphological transformation (DIMT) is introduced as a modular methodology to control the shape of sterically stabilized diblock copolymer nanoparticles and gain mechanistic insight into morphological transformations that occur during selective degradation of the methacrylic core-forming block. Notably, DIMT results in a sequential evolution in copolymer morphology from vesicles to worms to spheres. Transmission electron microscopy (TEM) and small-angle X-ray scattering (SAXS) studies enabled the construction of a predictive (pseudo)phase diagram. Furthermore, this new approach was also applied to the irreversible degelation of diblock copolymer worm gels, highlighting new opportunities to regulate material properties through depolymerization.