Summary: A highly asymmetric P2VP58‐PAA924‐PBMA48 double hydrophilic block terpolymer exhibits a rich phase behavior as a function of pH. In acidic media (pH 1) three compartment micelles with a positively charged outer corona are formed. At high pH, the above structure is transformed into a three‐dimensional transient network constituted of hydrophobic domains interconnected with negatively charged bridging chains (PAA chains). At even higher pH (14) the network is disrupted and finally exhibits a closed loop sol–gel–sol behavior.
AFM images of P2VP58‐PAA924‐PBMA48 micellar self assemblies deposited on mica.