A pH-responsive supramolecular network formed from gamma-cyclodextrin and linear poly(ethylene glycol)-blockpoly(ethyleneimine) (PEG-b-PEI) copolymers (see figure) by double-axle intrusion (DI) can modulate its rheological properties in response to pH changes. The formation of the DI system induces a drastic increase in the rheological properties even under very diluted conditions. The DI system shows significantly reduced viscoelastic properties at low pH.