Sulfur capture by limestone particles in a circulating fluidized bed is studied by modeling. Small particles are reactive but they have a short residence time depending on the separation efficiency of the cyclone. With large particles, the residence time is longer, but the rate and degree of sulfur capture are lower. Then the large particles removed in the bottom ash flow may have reached a lesser degree of conversion (from CaO to CaSO4), especially if the rate of attrition is low. The optimum particle size or particle-size distribution to minimize the limestone feed rate to achieve a given efficiency of sulfur capture is discussed. A methodology to calculate the optimum size is presented.