Limestone attrition by surface wear was studied during the flue gas desulfurization under simulated fluidized-bed (FB) oxyfiring conditions and hindered calcination. Bench-scale experimental tests were carried out using well-established techniques previously developed for the characterization of sulfation and attrition of sorbents in air-blown atmospheric FB combustors. The experimental limestone conversion and attrition results were compared with those previously obtained with the same limestone under simulated air-blown combustion conditions. The differences in the conversion and attrition extents and patterns associated with oxyfiring as compared to air-blown atmospheric combustion were highlighted and related to the different particle morphologies and thicknesses of the sulfate layer. It was noted that attrition could play an important role in practical circulating FB combustor operation, by effectively enhancing particle sulfation under both oxyfiring and air-blown combustion conditions.