Assessment of human exposure to atmospheric metals is a challenge, and mosses seem to be good biomonitors to help this purpose. Lacking roots, they are easy to collect and analyze. However, to our knowledge, no formal comparison was made between cadmium (Cd) measurements in Grimmia mosses and alternative forecasts of atmospheric Cd pollution as those produced by the CHIMERE chemistry transport model. This work aims at studying this link to improve further biomonitoring. We compare 128 Cd measurements in the cemetery mosses of Paris and Lyon metropolitan areas (France) to CHIMERE Cd atmospheric forecasts. The area to consider around the cemetery for the CHIMERE forecasts has been defined by Kendall rank correlations between both information sources—Cd in mosses and CHIMERE Cd forecasts—from different area sizes. Then, we fit linear models to those two data sets including step-by-step different sources of uncertainty. Finally, we calculate moss predictions to compare predictions and measurements in the two cities. The results show an apparent link between the Cd concentrations in mosses and CHIMERE Cd forecasts including in addition the same unique covariate, the moss support (grave or wall), in the two cities. However, this model cannot be directly transposed from region to region because the strength of the link appears to be regional.