A consecutive-reaction kinetic model for the sucrose-fed upflow anaerobic sludge bed (UASB) reactor that accounts for a layered structure of the granule and the mass fraction of methanogens (f) is proposed. When the UASB reactor was maintained at the volumetric loading rates (VLR) of 7.9–13.8 kg chemical oxygen demand (COD)/m3 d, the accumulated volatile fatty acids (VFAs) increased with increasing VLR, whereas the experimental f decreased with increasing VLR. This was primarily because methanogenesis was the ratelimiting step and the sucrose-fed granule was a layered structure. The calculated residual concentrations of sucrose and the intermediates VFAs using the layered-structure model are less deviated from the experimental measurements than those using the homogeneous-structure model. The calculated effectiveness factors for sucrose uptake and intermediates VFAs uptake (Z1; Z2) ranged from 0.18 to 0.35 and 0.65 to 0.96, respectively, indicating that the overall substrate (sucrose or intermediates VFAs) removal in the UASB reactor was diffusion-controlled, especially at the VLRs of 7.9–10.6. kgCOD/m3 d. This finding was also confirmed by the simulated concentration profiles of sucrose and VFAs in the UASB-granule. From the simulation results, the effect of internal mass transfer resistance on overall substrate (sucrose) removal should not be neglected, especially for a granule size of greater than 2.0mm.