This Perspective discusses the recent development of polymerization-induced self-assembly mediated by reversible addition–fragmentation chain transfer (RAFT) aqueous dispersion polymerization. This approach has become a powerful and versatile technique for the synthesis of a wide range of bespoke organic diblock copolymer nano-objects with controllable size, morphology, and surface functionality. These formulations are environmentally friendly and have potential applications such as novel Pickering emulsifiers, efficient microencapsulation vehicles, and sterilizable thermo-responsive hydrogels for the cost-effective long-term storage of mammalian cells. The key to this method is the use of RAFT polymerization to chain-extend a water-soluble polymer precursor with a water-immiscible monomer, resulting in an amphiphilic diblock copolymer that self-assembles in situ. This process can produce diblock copolymer nanoparticles in the form of spheres, worms, or vesicles, with the final morphology determined by the relative volume fractions of the hydrophilic and hydrophobic blocks. Aqueous dispersion polymerization is a versatile alternative to aqueous emulsion polymerization, involving the chain extension of a suitable water-soluble polymer to act as a steric stabilizer. This method is conducted using RAFT chemistry, which allows for the controlled polymerization of functional vinyl monomers while minimizing termination reactions. The use of RAFT aqueous dispersion polymerization has enabled the synthesis of various thermo-sensitive nanogels, with the ability to tune the morphology of the resulting nanoparticles by varying the packing parameter, P. The synthesis of diblock copolymer nano-objects has been demonstrated using various monomers, including N-isopropylacrylamide (NIPAM), N,N'-diethylacrylamide (DEAA), 2-methoxyethyl acrylate (MEA), 2-hydroxypropyl methacrylate (HPMA), and di(ethylene glycol)methyl ether methacrylate (DEGMA). These monomers form a relatively small subset of building blocks that fulfill the essential requirements for an aqueous dispersion polymerization formulation. The ability to control the morphology of the resulting nanoparticles has been demonstrated through the use of phase diagrams, which allow for the targeting of pure copolymer morphologies. The phase diagrams show that the final copolymer morphology is determined by the target DP of the core-forming block and the copolymer concentration. This has enabled the synthesis of various morphologies, including spheres, worms, and vesicles. The use of RAFT aqueous dispersion polymerization has also enabled the synthesis of thermoresponsive diblock copolymer worm gels, which exhibit reversible transitions between worm and sphere morphologies upon temperature changes. These gels have potential applications in biomedical fields, such as sterilization and microencapsulation. In addition, the synthesis of ABC triblock copolymer vesicles has been demonstrated, with the ability toThis Perspective discusses the recent development of polymerization-induced self-assembly mediated by reversible addition–fragmentation chain transfer (RAFT) aqueous dispersion polymerization. This approach has become a powerful and versatile technique for the synthesis of a wide range of bespoke organic diblock copolymer nano-objects with controllable size, morphology, and surface functionality. These formulations are environmentally friendly and have potential applications such as novel Pickering emulsifiers, efficient microencapsulation vehicles, and sterilizable thermo-responsive hydrogels for the cost-effective long-term storage of mammalian cells. The key to this method is the use of RAFT polymerization to chain-extend a water-soluble polymer precursor with a water-immiscible monomer, resulting in an amphiphilic diblock copolymer that self-assembles in situ. This process can produce diblock copolymer nanoparticles in the form of spheres, worms, or vesicles, with the final morphology determined by the relative volume fractions of the hydrophilic and hydrophobic blocks. Aqueous dispersion polymerization is a versatile alternative to aqueous emulsion polymerization, involving the chain extension of a suitable water-soluble polymer to act as a steric stabilizer. This method is conducted using RAFT chemistry, which allows for the controlled polymerization of functional vinyl monomers while minimizing termination reactions. The use of RAFT aqueous dispersion polymerization has enabled the synthesis of various thermo-sensitive nanogels, with the ability to tune the morphology of the resulting nanoparticles by varying the packing parameter, P. The synthesis of diblock copolymer nano-objects has been demonstrated using various monomers, including N-isopropylacrylamide (NIPAM), N,N'-diethylacrylamide (DEAA), 2-methoxyethyl acrylate (MEA), 2-hydroxypropyl methacrylate (HPMA), and di(ethylene glycol)methyl ether methacrylate (DEGMA). These monomers form a relatively small subset of building blocks that fulfill the essential requirements for an aqueous dispersion polymerization formulation. The ability to control the morphology of the resulting nanoparticles has been demonstrated through the use of phase diagrams, which allow for the targeting of pure copolymer morphologies. The phase diagrams show that the final copolymer morphology is determined by the target DP of the core-forming block and the copolymer concentration. This has enabled the synthesis of various morphologies, including spheres, worms, and vesicles. The use of RAFT aqueous dispersion polymerization has also enabled the synthesis of thermoresponsive diblock copolymer worm gels, which exhibit reversible transitions between worm and sphere morphologies upon temperature changes. These gels have potential applications in biomedical fields, such as sterilization and microencapsulation. In addition, the synthesis of ABC triblock copolymer vesicles has been demonstrated, with the ability to