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Due to their self-assembled nature, wormlike micelles (WLMs) offer an ideal platform for the design of stimulus-responsive or ‘smart’ materials. By using amphiphilic molecules that alter their configurations, and thus their packing, in response to environmental triggers such as pH, light, or temperature, the morphology of the resulting aggregates can be switched ‘on’ and ‘off’, resulting in drastic changes of the viscoelasticity of the solutions, thus an effective sol–gel transition. This chapter summarizes the results published in this field over the last few years, reporting in particular on more recent types of triggers (such as CO2) and highlighting the relationship between molecular architecture, microstructure, and macroscopic viscoelasticity.

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