Designing supramolecular pastes by controlling host–guest dynamics in reconfigurable networks

Stimuli-responsive phase transitions endow smart systems with adaptive functionalities, yet reversible paste-to-gel transitions remain largely unexplored. Here, we report a protonated trianglamine (TA)-based supramolecular paste, in which competitive supramolecular interactions-host-guest binding and electrostatic forces-drive the formation of a dynamic TA-clay-polymer ternary network with paste-like rheology. The material exhibits reversible paste-to-gel transitions under mild thermal stimuli, enabling shape reprogramming, temperature-triggered self-healing, and shape fixation. DFT calculations and molecular simulations reveal the molecular basis of the host-guest interactions in guiding network dynamics and healing behavior. Furthermore, incorporating graphene as conductive filler renders the paste functions as a stretchable, self-healing conductive wire, with potential in flexible electronics and responsive devices. This work introduces supramolecular pastes as a versatile class of smart materials that go beyond traditional hydrogels in structural adaptability and multifunctionality.