Paired indoor and outdoor concentrations of fine and coarse particulate matter (PM), PM2.5 reflectance [black carbon(BC)], and nitrogen dioxide (NO2) were determined for sixteen weeks in 2008 at four elementary schools (two in high and two in low traffic density zones) in a U.S.–Mexico border community to aid a binational health effects study. Strong spatial heterogeneity was observed for all outdoor pollutant concentrations. Concentrations of all pollutants, except coarse PM, were higher in high traffic zones than in the respective low traffic zones. Black carbon and NO2 appear to be better traffic indicators than fine PM. Indoor air pollution was found to be well associated with outdoor air pollution, although differences existed due to uncontrollable factors involving student activities and building/ventilation configurations. Results of this study indicate substantial spatial variability of pollutants in the region, suggesting that children’s exposures to these pollutants vary based on the location of their school.