Recent evidence has linked air pollution with frailty, yet little is known about the role of NO2 in this association. Our aim was to assess the association between frailty and NO2 air concentrations in Mexican older adults. We used georeferenced data from the population-based Nutrition and Health Survey in Mexico (NHNS) 2021, representative of national and subnational regions, to measure a frailty index based on 31 health deficits in adults aged 50 and older. Air pollution due to NO2 concentrations was estimated from satellite images validated with data from surface-level stations. Maps were produced using Jensen's Natural break method. The association of frailty and NO2 concentrations was measured using the frailty index (multivariate fractional response logit regression) and a frailty binary variable (frailty index [FI] ≥0.36, multivariate logit regression). There was a positive and significant association of the frailty index with the NO2 concentrations, adjusting for age, sex, urban and rural area, years of education, socioeconomic status, living arrangement, particulate matter smaller than 2.5 microns, and indoor pollution. For each standard deviation increase in NO2 concentrations measured 10 years before the survey, the odds of being frail were 15% higher, and the frailty index was 14.5% higher. The fraction of frailty attributable to NO2 exposure ranged from 1.8% to 23.5% according to different scenarios. Frailty was positively associated with exposure to NO2 concentrations. Mapping frailty and its associated factors like NO2 air concentrations can contribute to the design of targeted pro-healthy aging policies.