To meet modern society’s requirements for sustainability and environmental protection, innovative and smart surface coatings are continually being developed to improve or impart surface functional qualities and protective features. These needs regard numerous different sectors, such as cultural heritage, building, naval, automotive, environmental remediation and textiles. In this regard, researchers and nanotechnology are therefore mostly devoted to the development of new and smart nanostructured finishings and coatings featuring different implemented properties, such as anti-vegetative or antibacterial, hydrophobic, anti-stain, fire retardant, controlled release of drugs, detection of molecules and mechanical resistance. A variety of chemical synthesis techniques are usually employed to obtain novel nanostructured materials based on the use of an appropriate polymeric matrix in combination with either functional doping molecules or blended polymers, as well as multicomponent functional precursors and nanofillers. Further efforts are being made, as described in this review, to carry out green and eco-friendly synthetic protocols, such as sol–gel synthesis, starting from bio-based, natural or waste substances, in order to produce more sustainable (multi)functional hybrid or nanocomposite coatings, with a focus on their life cycle in accordance with the circular economy principles.