Four methods for cleaning the limestone facades on what was originally the Workers' Hospital are analyzed in this paper. Due to the pollution in the surrounding air, just twenty years after a prior cleaning operation, sulfate crusts had developed on the entire stone surface of the building. The gypsum mortar used in the original masonry constituted an additional source of sulfur. Limestone is a traditional building material in Madrid and surroundings. The petrography, mineralogy and petrophysical properties of the biomicrite, pelmicrite and biopelmicrite varieties identified in the hospital walls were determined. An analysis of the black layer on the stone surface showed that it consisted primarily of sulfate crusts. The cleaning methods tested were alkaline gels (sodium hydroxide and potassium hydroxide), pressurized hot water, glass bead blasting and latex peeling. The criteria for assessing the effectiveness and potential dangerousness of the various cleaning systems included changes in the chromatic parameters of the clean stone, as well as formation of alteration products (i.e., salts) and modification of the stone surface. The stones cleaned with the three most effective methods as well as the rain-washed stone used as a reference were washed to generate an artificial runoff. The drain water collected was analyzed to determine possible cleaning process by-products. The method found to be most effective and alter the stone surface the least was glass bead blasting, particularly after adjustment of the bead size and pressure conditions used for the test.