Worldwide there is concern about the continuing release of persistent organic pollutants (POPs) into the environment. In this study we review the application of mosses as biomonitors of atmospheric deposition of POPs. Examples in the literature show that mosses are suitable organisms to monitor spatial patterns and temporal trends of atmospheric concentrations or deposition of POPs. These examples include polycyclic aromatic hydrocarbons (PAHs), polychlorobiphenyls (PCBs), dioxins and furans (PCDD/Fs), and polybrominated diphenyl ethers (PBDEs). The majority of studies report on PAHs concentrations in mosses and relative few studies have been conducted on other POPs. So far, many studies have focused on spatial patterns around pollution sources or the concentration in mosses in remote areas such as the polar regions, as an indication of long-range transport of POPs. Very few studies have determined temporal trends or have directly related the concentrations in mosses with measured atmospheric concentrations and/or deposition fluxes.