The flue gas desulfurization (FGD) process is currently the most effective process utilized to remove sulfur dioxide from stack gases of coal-fired plants. However, FGD systems use a lot of limestone as desulfurizing agent. In this study, we use limestone sludge, which is a by-product of the steel industry, to replace the desulfurizing agent of the FGD system. The limestone particle size is found to be unrelated to the desulfurizing rate; the gypsum purity, however, is related. Limestone sludge mixes with limestone slurry delivered at a constant rate in a desulfurizing agent with organic acid are expected to lead to a high desulfurization efficiency and high quality by-product (gypsum).