Lime mortars have been commonly used in historical buildings since ancient times. The progressive deterioration of these mortars by air pollution and other environmental causes hinders the assessment of the original composition. The weakening of the mortar structure is due to dissolution and formation of calcium sulphate layers because of the interaction with SOx gaseous pollutants. Also, pollution particles can be incorporated to the mortar because of dissolution by rainwater or runoff. Scanning Electron Microscopy (SEM) studies allow us to distinguish allochthonous and autochthonous micro- and nanoparticles in order to identify original intact plasters. By comparing these intact to deteriorated mortars from both air polluted and non-polluted areas it is possible to indentify and preserve the original mortar composition as a key step to project future façade cleaning and restorations.