Coal is the most important nonrenewable energy source of fossil origin. It is also the most common fuel in thermal power plants. However, during coal incineration in power plants, high sulfur content of coal poses serious environmental problems owing to sulfur dioxide emission. We studied the application of microbial methods for removal of sulfur from three types of high sulfur coals—two samples collected from Assam and Rajasthan in India and one from Libiaz, Poland. These coal samples were desulfurized using indigenous Acidithiobacillus sp. After investigation of the effect of various parameters, the conditions optimized for the maximum removal of total sulfur (91.87% for lignite, 63.13% for Polish coal, and only 9.44% for Assam coal) were as follows: initial pH of 1.5 (2.5 in the case of Assam coal), particle size of 45 μ, pulp density of 2% (w/v), incubation period of 30 d at −35°C in presence of 44.2 g/L of ferrous sulfate in the media with shaking at 140 rpm. Poor removal of sulfur in the case of Assam coal was owing to extensive precipitation of jarosites. In addition, the sulfur in Assam coal is mostly found in organic form, which is difficult to remove with Acidithiobacillus sp. The removal of sulfur from the three coal samples was demonstrated with photomicrographic studies.