This Brief offers a contemporary overview of smart surfactants, detailing various triggers that lead to the formation of wormlike micelles or alter surfactant aggregate morphology. It integrates chemistry, physics, polymer science, and nanotechnology, focusing on the design, formulation, and processing of intelligent viscoelastic surfactant solutions. The initial chapter discusses the self-assembly of surfactants into viscoelastic wormlike micellar solutions, akin to polymer solutions. Subsequent chapters explore how responses to specific triggers—such as temperature, light, pH, CO2, redox reactions, and hydrocarbons—result in macroscopic rheological changes. The final chapter highlights applications of these viscoelastic assemblies in oil and gas production, drag reduction, biomaterials, cleaning processes, and electrorheological and photorheological fluids. The Brief concludes with comments and perspectives. It targets chemists, physicists, chemical engineers, and nano-scientists engaged in surfactant self-assemblies and applications, as well as graduate students in physical chemistry. The authors include Yujun Feng, Ph.D., a professor at the State Key Laboratory of Polymer Materials Engineering in China; Zonglin Chu, Ph.D., a post-doctoral fellow at the University of Zürich; and Cécile A. Dreiss, Ph.D., a senior lecturer at King’s College London.
