The atmosphere is an important pathway for microplastic (MP) transport; however, observations are limited, as traditional sampling methods are generally labor-intensive. Biological monitors (biomonitors) have been widely used as a simple alternative to determine the abundance or presence of anthropogenic pollutants. Here, we compared the effectiveness of co-located lichen and moss species as biomonitors of the atmospheric deposition of microplastics. Samples of the epiphytic lichen Evernia prunastri and the epigeic moss Pseudoscleropodium purum were collected from five remote areas of central Italy. A total of 154 MPs were found across all samples, 93.5% of which were fibers and 6.5% were fragments. The accumulation of MPs for lichens (range of 8–12 MP/g) was significantly lower than for mosses (12–17 MP/g), which might be related to their structural characteristics or habitat positions (epiphytic versus epigeic). Nonetheless, higher accumulation facilitates analytical determination and provides greater separation from the limit of detection, suggesting that mosses are preferred over lichens for studying the deposition of airborne MPs. This study further suggests that biomonitoring may be an effective tool to assess the spatial distribution of atmospheric microplastics, which is a key requirement for the development of waste mitigation policies. Keywords: atmosphere; biomonitoring; lichen; moss; microplastics; Italy.