Dual Thermo- and pH-Responsive <i>N</i>-Cyanomethylacrylamide-Based Nano-Objects Prepared by RAFT-Mediated Aqueous Polymerization-Induced Self-Assembly

We report the straightforward synthesis of dual stimuli-responsive nano-objects using a RAFT-mediated polymerization-induced self-assembly process in water. The key to complex and tunable responsiveness was copolymerization N-cyanomethylacrylamide, providing upper critical solution temperature-type polymers, with pH-sensitive monomer (acrylic acid, AA). Not only core block length but also AA content slight changes degree ionization polymerization medium (?AA,0) had great impact on particle morphology. Generally, higher contents favored formation spherical nano-objects, while low ?AA,0 led higher-order morphologies. demonstrated that exhibited temperature. Progressively increasing post-polymerization units incorporated copolymer (?AA) triggered morphological transitions. Remarkably, single composition formed well-defined vesicles, worms, spheres eventually dissociated into individual chains. Temperature-dependent small-angle X-ray scattering analyses evidenced thermo-responsive behavior, which depended ?AA. For some compositions, we observed both cloud point clearing point, attributed secondary aggregates chain dissolution, respectively.