The extent of hydrogen spillover on two different Pd-based catalysts supported on mesoporous SBA-15 and MCM-41 is quantitatively predicted using a crystallite-scale model, which considers the effect of size and location of crystallites, metal-support interfacial contact, and diffusivity of the adsorbed species on the support surface. The developed model, in combination with a fixed-bed reactor model predicts that in the absence of any reductant in the feed, the NO conversion is higher (= 37 %) on the SBA-15 supported catalyst as compared to 25 % on MCM-41, which is consistent with the reported data in the literature. The difference in the catalytic activity is ascribed to the different spillover rates of hydrogen on SBA-15 and MCM-41, which is further correlated to the fraction of Pd crystallites present in the support channels. The model is also used to study the effect of cycle time, H-2 concentration, Pd dispersion, and Pd loading on NO reduction under cyclic conditions. Consistent with the literature findings, the model predicts that the Pd surface area and the metal-support interfacial contact increase with an increase in the Pd loading and dispersion, which result in higher spillover and hence increase the NO conversion. Even though the present model has been developed for the H-2-SCR system, it can also be extended to other catalytic systems where spillover effects are significant.