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The formation of films of molecules at the water–air interface has provided stunning examples of molecular assembly, novel ways to study interactions between monolayers and adsorpts dissolved in the water phase, and an unparalleled versatility for the formation of multilayers using the Langmuir–Blodgett technique. Instinct might make one think that there is little new in the area; far from it. New systems, techniques and science are ever increasing as the versatility of layers on liquids is exploited for new discoveries in nanoscience. The intermolecular forces that bring about self-assembly of surfactants at the water–air interface and that determine the domain morphologies will be presented, and the main families of supramolecular phenomena and structures formed on water will be discussed, from classical surfactants to molecular hosts and their interactions with guests. The utility of the “lift” or Langmuir–Schaefer method for picking up supramolecular structures will be demonstrated as a unique way to transfer monolayers onto solid substrates, as will the more recent “scooping up” method. Contemporary examples and potential routes for new knowledge for supramolecular science, medicine and electronics will be discussed. The use of other liquids—such as mercury—and the uniqueness of each interface will be presented.

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