One of the main problems connected to the conservation of street art is the selective removal of overlying undesired graffiti, i.e., drawings and tags. Unfortunately, selective and controlled removal of graffiti and overpaintings from street art is almost unachievable using traditional methodologies. Recently, the use of nanofluids confined in highly retentive pHEMA/PVP semi-interpenetrated polymer networks was proposed. Here, we report on the selective removal of acrylic overpaintings from a layer of acrylic paint on mortar mockups in laboratory tests. The results of the cleaning tests were characterized by visual and photographic observation, optical microscopy, and FT-IR microreflectance investigation. It was shown that this methodology represents a major advancement with respect to the use of nonconfined neat solvents.