In the present work, a reaction of sulfur removal and simulation of desulfurization based on the grain model and two-phase theory were studied using natural manganese ore (NMO) as a sorbent in a continuous fluidized bed reactor. The effect of desulfurization was investigated through the grain model considered the change of pore structure as a function of desulfurization time, particle size of NMO, and diffusion velocity of SO2 in the pores. Among these parameters, the diffusion of SO2 in the pores of NMO was the most important factor. Moreover, the reaction of sulfur removal and desulfurization in a continuous fluidized bed reactor using NMO as a sorbent could be well predict through the grain model and two-phase theory, respectively.