BACKGROUND: Previous studies of short-term ambient air pollution exposure and asthma morbidity in the United States have been limited to a small number of cities and/or pollutants and with limited consideration of effects across ages. OBJECTIVES: To estimate acute age group-specific effects of fine and coarse particulate matter (PM), major PM components, and gaseous pollutants on emergency department (ED) visits for asthma during 2005-2014 across the United States. METHODS: We acquired ED visit and air quality data in regions surrounding 53 speciation sites in 10 states. We used quasi-Poisson log-linear time-series models with unconstrained distributed exposure lags to estimate site-specific acute effects of air pollution on asthma ED visits overall and by age group (1-4, 5-17, 18-49, 50-64, and 65+ y), controlling for meteorology, time trends, and influenza activity. We then used a Bayesian hierarchical model to estimate pooled associations from site-specific associations. RESULTS: Our analysis included 3.19 million asthma ED visits. We observed positive associations for multiday cumulative exposure to all air pollutants examined [e.g., 8-d exposure to PM2.5: rate ratio of 1.016 with 95% credible interval (CI) of (1.008, 1.025) per 6.3-µg/m3 increase, PM10-2.5: 1.014 (95% CI: 1.007, 1.020) per 9.6-µg/m3 increase, organic carbon: 1.016 (95% CI: 1.009, 1.024) per 2.8-µg/m3 increase, and ozone: 1.008 (95% CI: 0.995, 1.022) per 0.02-ppm increase]. PM2.5 and ozone showed stronger effects at shorter lags, whereas associations of traffic-related pollutants (e.g., elemental carbon and oxides of nitrogen) were generally stronger at longer lags. Most pollutants had more pronounced effects on children (<18 y old) than adults; PM2.5 had strong effects on both children and the elderly (>64 y old); and ozone had stronger effects on adults than children. CONCLUSIONS: We reported positive associations between short-term air pollution exposure and increased rates of asthma ED visits. We found that air pollution exposure posed a higher risk for children and older populations. https://doi.org/10.1289/EHP11661.