Liquid-liquid interfaces offer highly controlled, flexible, and adaptable platforms for precise molecular assemblies, enabling the construction of sophisticated functional materials. Interfacial assemblies of specific nanoparticles (NPs) and ligands can alter their physicochemical states under external stimuli, leading to macroscopic dynamic transformations at the interface. This Review summarizes and analyzes the recent advances of the assembly and disassembly behaviors of various stimuli-responsive nanoparticle surfactants (NPSs) at liquid-liquid interfaces, focusing on their responsive behaviors when exposed to external stimuli and the interaction forces between interfacial molecules. Additionally, we outline recent advancements in applications such as reconfigurable all-liquid devices, all-liquid 3D printing, and chemical reaction platforms. Finally, we discuss current challenges and future prospects for the development of applications in this rapidly evolving field.
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