Organisms living at the stone–air interface are expected to be affected by changes in the atmospheric composition due to greenhouse gases emissions. Increased CO2 concentrations may particularly affect phototrophic microorganisms that colonize stone cultural heritage and form subaerial biofilms. However, little is known about the effects of the environmental changes on microorganisms that colonize stone and the consequences for cultural heritage conservation. In the present study, we investigated how an increase in inorganic carbon concentration affected the development of a subaerial biofilm composed by the cyanobacterium Synechocystis sp. PCC 6803 grown on granite. For this purpose, we established two experiments on biofilm formation, with and without addition of inorganic carbon to the growth medium. Higher concentrations of carbon promoted biofilm growth and increased the concentrations of the photosynthetic pigments chlorophyll a and carotenoids on granite surface, potentially exacerbating the aesthetic impact of these biofilms on stone-made cultural heritage. However, the extracellular polysaccharides produced were not significantly affected by carbon availability, so that physical stone biodeterioration might not be increased by the cyanobacterial matrix. The findings provide valuable data on how the existing global change scenario might affect organisms inhabiting stone cultural heritage and encourage to develop new sustainable treatments and methodologies to prevent biodeterioration and thus preserve stone cultural heritage.