Unauthorised graffiti is a challenge in urban environments, affecting railway structures, stations, tracks, and vehicles. Inefficient cleaning methods increase the costs and downtime of railcars, limiting passenger transport. In turn, they are harmful to the operator’s health and the environment, due to the VOCs they release. This study focuses on the feasibility of dry-ice blasting, replacing carbon dioxide with ambient air as an innovative and sustainable solution to remove graffiti from rail vehicles. Experimental tests have been carried out with 13 different aerosols, controlling the temperature (<−80 °C), pressure (up to 3 bar), projection distance (0.5 cm) and exposure times (30″/1′/2′/4′/6′/8′/++). The results showed that ultra-freezing with ambient air preserved the integrity of the support materials and altered the topography, colourimetry and adhesion of the aerosols tested, achieving the total removal of one of the paints. Preliminary results suggest that ultra-freezing with ambient air could be a viable and sustainable solution for graffiti removal on railway structures, transferable to other urban environments.