Calendering of coated paper leads to a brightness decrease. The mechanism for this is not clear, although it has been discussed in the past. One common explanation is that the porosity of the coating layer decreases and hence scattering. By comparing simulated and measured results this paper shows that modifications of the surface properties account for the brightness decrease of GCC coated substrates with calendering. The effect of a deformable cartonboard substrate is investigated here and compared to a less deformable plastic film substrate. From simulations based on a two-layer Kubelka-Munk model, it is shown that the brightness decrease of the cartonboard due to calendering has a negligible contribution to the brightness decrease of the coated cartonboard. The brightness decrease was similar for coated plastic film and coated cartonboard. The thickness of GCC coated plastic films was not affected by calendering irrespectively of the pigment and latex size distribution. Monte Carlo light scattering simulations, taking into account the measured decrease of surface microroughness and increased effective refractive index, showed that surface modifications accounted for most of the observed brightness decrease of the GCC coated substrate, whereas the bulk scattering and absorption coefficients were not affected by calendering. It is also shown that the scattering coefficient is significantly dependent on the coat weight whereas the physical absorption coefficient is not.