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Films prepared by the sequential treatment of surfaces with small molecules or polymeric macromolecules, of charged or neutral character, can have behaviour that is completely different to the materials prepared in bulk. The approach requires the formation of non-covalent complexes between surface-immobilised ions or moieties and part of a molecule bearing multiple recognition sites in the overlying medium. The templating surface for the film is crucial in the early stages of formation of the multilayers, which are formed in a stepwise way with the requirement of self-limiting growth. The routes used to prepare the surface-based supramolecular systems can give unique systems that can be dense or porous, and in controlled ways. The preparation of polyelectrolyte films that employ principally electrostatic interactions with a strong entropic component at play in the assembly will be shown, and their structure and properties presented and compared with the layer-by-layer approach to supramolecular films based on weaker interactions. The preparation of coordination frameworks, the metal–organic frameworks, on surfaces is a unique pathway to control assembly and orientation of this kind of material, at least for the formation of quite thin films. The use of the different paradigms for assembly on surfaces from solution affords a fascinating toolkit for the preparation of supramolecular composite film materials, which will be discussed to show the potential applications of these systems.

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