Abstract

Supramolecular hydrogels can spontaneously undergo syneresis through fibre–fibre interactions and expel significant amounts of water upon aging. In this process, the hydrophobicity of fibres which regulates the 3D‐rearrangement of the self‐assembled structures during syneresis is important. Here, we show that we can control the hydrophobic microenvironment of gels by incorporating organic salts into the co‐assembled gel fibres thereby enabling control of the macroscopic gel volume phase transition.

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