The application of a new class of organogels as cleaning tools for painted surfaces is described. It combines some of the most attractive features of cleaning liquids and normal gels while diminishing the deleterious characteristics of both. Thus, the ‘latent’ gellant, polyethyleneimine (PEI), reacts with CO₂ at room temperature in solutions of several organic liquids to produce an ammonium carbamate form (PEICO₂). This charged species organizes itself into 3D polymer networks which immobilize the liquids as gels. The properties of the original solution (i.e. a free-flowing liquid) are re-established immediately after addition of a small amount of a weak acid which displaces the CO₂ molecules and makes the PEI chains positively charged. The visual changes are substantiated by rheological analyses. Results from analytical tests to determine the utility of these gels as cleaning tools for painted surfaces of historical and artistic interest, have been obtained from contact angle and FTIR measurements as well as visual comparisons of the surfaces before and after application of the gels. The analyses indicate that the PEICO₂-based organogels were very effective in removing different surface patinas from painted supports. A surface layer of dammar was completely removed from a test canvas with oil paint, an aged painting from the XIX century, and a XV century oil-on-wood panel attributed to Mariotto di Cristoforo. Finally, a surface acrylic polymeric resin (used in a restoration performed during the 1960s) was also successfully removed from Renaissance wall paintings decorating the Santa Maria della Scala Sacristy in Siena, Italy. The isothermally rheoreversible gel approach described in this work represents a new, highly versatile, and very efficient method for removing aged surface patinas from works of art.