LAUSR

Wormlike micelles, which are flexible elongated aggregates formed by the self‐assembly of surfactant molecules in aqueous solutions, have been widely applied in various fields because of their unique morphology and dynamic characteristics. However, the studies on the unsaturation of tails, particularly in solutions of double‐tailed surfactants, remain limited. This study examines the influence of the chemical structure of hydrophobic tails on the formation and rheological properties of wormlike micelles. Two types of double‐tailed surfactants with distinct tail structures, one containing double bonds and the other without, were designed and synthesized. The results show that introducing double bonds into the tail significantly affects the formation mechanism and physicochemical properties of wormlike micelles. Wormlike micelles formed from surfactants with double bonds exhibit enhanced rheological properties and viscoelastic behavior. This study enhances the understanding of the relationship between surfactant tail structure and micelle behavior. It provides theoretical and experimental support for the future design of efficient surfactants and offers new perspectives and technical guidance for their application in enhanced oil recovery, drug delivery, and environmental remediation. Future studies could explore the behavior of structurally diverse double‐tailed surfactants in more complex solutions, thus expanding their potential applications across broader fields.