Green nanostructured fluids (GNFs), specifically water‐in‐oil nanoemulsions (w/o NEs), were investigated as professional “brush on, wipe off” nanodetergents for the effective removal of various challenging graffiti coatings. The efficacy of the advanced nanodetergents in eradicating resilient graffiti coatings was evaluated using various methods to assess the surface properties of forming graffiti coatings. The surface properties of these coatings were examined by assessing their wettability by water, surface free energy, and topography to obtain information on the intermolecular interactions with the nanodetergent during the wetting and graffiti removal process. Our findings revealed significant variations in the coating removal rate and efficacy of green nanostructured fluids, which are stabilized using surfactants derived from saccharides or amino acids. A water‐in‐oil nanoemulsion, stabilized by caprylyl/capryl glucoside, demonstrated exceptional efficiency at cleaning graffiti paints based on alkyd resin and containing various additives such as nitrocellulose or bitumen, from any hard surface within a short time period. However, a w/o NE, stabilized by sodium cocoyl glycinate, also showed effective removal of graffiti paints containing durable bitumen, albeit at a slower rate on. These green nanostructured fluids can be used as specific nanodetergents for the comprehensive removal of various graffiti coatings, but require a specified action time to prevent damage to the original substrate beneath the paint coating.