This perspective discusses the recent development of polymerization-induced self-assembly (PISA) mediated by reversible addition–fragmentation chain transfer (RAFT) aqueous dispersion polymerization. This technique has become a powerful and versatile method for synthesizing a wide range of bespoke organic diblock copolymer nano-objects with controllable size, morphology, and surface functionality. The environmentally friendly nature of these formulations makes them promising for various applications, such as Pickering emulsifiers, micro-encapsulation vehicles, and thermo-responsive hydrogels for long-term mammalian cell storage. The introduction highlights the historical context of block copolymer self-assembly, from the discovery of living polymerizations to the emergence of interdisciplinary research in polymer chemistry, physics, and engineering. It emphasizes the challenges in synthesizing well-defined block copolymer nanoparticles in concentrated aqueous solutions and the progress made by Charleux and colleagues using emulsion polymerization. The perspective then delves into the details of aqueous dispersion polymerization, focusing on the use ofRAFT chemistry. This method involves chain extension of a water-soluble polymer with a water-immiscible monomer, leading to the formation of stable colloidal dispersions. The authors discuss the selection of suitable monomers, such as N-isopropylacrylamide, N,N'-diethylacrylamide, and 2-hydroxypropyl methacrylate, and their impact on the resulting copolymer morphology. The article also explores the synthesis of thermo-responsive nanogels using RAFT aqueous dispersion polymerization, highlighting the importance of pH and temperature in controlling the morphology of the resulting nanoparticles. It describes the preparation of various morphologies, including spheres, worms, and vesicles, and the factors influencing their formation, such as the packing parameter and the degree of polymerization. The authors further discuss the use of phase diagrams to target specific copolymer morphologies and the potential for cost-effective formulations. They explore the synthesis of ABC triblock copolymer vesicles and their applications in Pickering emulsions and drug delivery systems. The article concludes with a discussion on future research directions, including the development of pH-responsive nanoparticles and the theoretical framework for PISA, emphasizing the importance of advanced characterization techniques like SAXS and cryo-TEM.This perspective discusses the recent development of polymerization-induced self-assembly (PISA) mediated by reversible addition–fragmentation chain transfer (RAFT) aqueous dispersion polymerization. This technique has become a powerful and versatile method for synthesizing a wide range of bespoke organic diblock copolymer nano-objects with controllable size, morphology, and surface functionality. The environmentally friendly nature of these formulations makes them promising for various applications, such as Pickering emulsifiers, micro-encapsulation vehicles, and thermo-responsive hydrogels for long-term mammalian cell storage. The introduction highlights the historical context of block copolymer self-assembly, from the discovery of living polymerizations to the emergence of interdisciplinary research in polymer chemistry, physics, and engineering. It emphasizes the challenges in synthesizing well-defined block copolymer nanoparticles in concentrated aqueous solutions and the progress made by Charleux and colleagues using emulsion polymerization. The perspective then delves into the details of aqueous dispersion polymerization, focusing on the use ofRAFT chemistry. This method involves chain extension of a water-soluble polymer with a water-immiscible monomer, leading to the formation of stable colloidal dispersions. The authors discuss the selection of suitable monomers, such as N-isopropylacrylamide, N,N'-diethylacrylamide, and 2-hydroxypropyl methacrylate, and their impact on the resulting copolymer morphology. The article also explores the synthesis of thermo-responsive nanogels using RAFT aqueous dispersion polymerization, highlighting the importance of pH and temperature in controlling the morphology of the resulting nanoparticles. It describes the preparation of various morphologies, including spheres, worms, and vesicles, and the factors influencing their formation, such as the packing parameter and the degree of polymerization. The authors further discuss the use of phase diagrams to target specific copolymer morphologies and the potential for cost-effective formulations. They explore the synthesis of ABC triblock copolymer vesicles and their applications in Pickering emulsions and drug delivery systems. The article concludes with a discussion on future research directions, including the development of pH-responsive nanoparticles and the theoretical framework for PISA, emphasizing the importance of advanced characterization techniques like SAXS and cryo-TEM.