Nanostructured Multiphase Condensation of Complex Coacervates in Polymerization-Induced Electrostatic Self-Assembly.

We present the nanostructured multiphase condensation of complex coacervates in the dynamic evolving aqueous medium of liquid-liquid phase separation driven polymerization-induced electrostatic self-assembly (LLPS-PIESA). We show that the parent droplets evolve into nanostructured coacervate-in-coacervate multiphase condensates with diverse morphologies, such as dandelions, worms, lamellae, vesicles, and vesicle polymers, upon the kinetically dictated recruitment of anionic free chains, cationic growing chains, and nascent clusters from the dynamic evolving aqueous medium of LLPS-PIESA, under the interplay of electrostatic and arginine-like salt bridge interactions.