摘要： Using the host-guest molecular recognition at the oil-water interface, a new-type photo-responsive nanoparticle surfactant (NPS), is designed and prepared to structure liquids. With the help of a polymeric surfactant, the interfacial host-guest interactions can be significantly enhanced, leading to a rapid formation and assembly of a NP monolayer, and offering sufficient binding energy to hold the NPs in a jammed state. The assembly of the NPSs can be reversibly manipulated via a photo-switchable jamming to unjamming transition, endowing the interface, as well as the macroscopic assemblies, with responsiveness to the external trigger (photons). This study, for the first time, opens the pathway for the construction of multi-responsive, structured all-liquid systems by introducing host?guest chemistry, showing promising potential applications in encapsulation, delivery systems, and unique microfluidic devices.