The monitoring of atmospheric nitrogen deposition is necessary considering that this kind of environmental pollution is among the leading causes of global biodiversity loss. However, deploying and operating monitoring networks can be cost-prohibitive; the use of naturally occurring biomonitors can be a viable alternative for characterizing such nitrogenous pollution, with bryophytes being of particular promise. For instance, a previous dose-response greenhouse experiment evaluating potential biomonitors of different life-forms revealed that the activities of the enzymes phosphomonoesterase and nitrate reductase respond linearly to simulated nitrogen deposition for the generalist neotropical moss Braunia secunda. The present work is the field validation of B. secunda and Leptodontium pungens, a specialist of oak forests, as biomonitors of nitrogen deposition. Moss samples were collected during the 2009 dry and rainy seasons from fir and oak forests at “low-pollution” or “high-pollution” sites within the Valley of Mexico, where the megalopolis of Mexico City is located, and transported to the laboratory for colorimetric determinations of enzymatic activity. The phosphomonoesterase activity was consistently higher for both mosses from the high-pollution sites than for the low-pollution sites, while the nitrate reductase had a lower activity for the plants collected from the high-pollution sites. These results suggest that the proposed biomonitors are appropriate for the region of study.