This research presents a study of environmental monitoring at different sampling sites from the Metropolitan Area of the Valley of Toluca (MAVT), Mexico, using mosses (Leskea angustata(Tayl.) andFabronia ciliaris(Brid.)) and soil samples. The epiphytic mosses and soils were sampled in two campaigns within two periods of the year, a rainy and dry-cold season. The selected sampling sites included urban regions (UR), transitional regions (TR), and protected natural areas (PA). The samples were analyzed by the Instrumental Neutron Activation Analysis (INAA) to determine As, Cr, Hg, and Se principally. However, due to the versatility of the analytic technique used, other elements including Cs, Co, Sc, Sb, Rb, Ce, La, Eu, and Yb were also detected. Statistical analysis (As, Cr, Hg, and Se) was carried out with principal components and cluster analysis methods; this revealed that a good correlation exists between metal content in mosses and the degree of pollution in the areas sampled. The obtained results in mosses showed that the concentrations of As, Cr, Co, Cs, Rb, Ce, La, and Yb increased with respect to the concentrations obtained during the first sampling, whereas Se, Sc, Sb and Eu, concentrations were decreased. For As and Hg, the concentrations were similar in both sampling periods. The soil samples present the most significant concentration.