Megacities can experience high levels of fine particulate matter (PM2.5) pollution linked to ammonia (NH3) mainly emitted from agricultural activities. Here, we investigate such pollution in the cities of Paris, Mexico, and Toronto, each of which have distinct emission sources, agricultural regulations, and topography. Ten years of measurements from the infrared atmospheric sounding interferometer (IASI) are used to assess the spatiotemporal NH3 variability over and around the three cities. In Europe and North America, we determine that temperature is associated with the increase in NH3 atmospheric concentrations with a coefficient of determination (r2) of 0.8 over agricultural areas. The variety of the NH3 sources (industry and agricultural) and the weaker temperature seasonal cycle in southern North America induce a lower correlation factor (r2=0.5). The three regions are subject to long-range transport of NH3, as shown using HYSPLIT cluster back trajectories. The highest NH3 concentrations measured at the city scale are associated with air masses coming from the surrounding and north/northeast regions of Paris, the south/southwest areas of Toronto, and the southeast/southwest zones of Mexico City. Using NH3 and PM2.5 measurements derived from IASI and surface observations from 2008 to 2017, annually frequent pollution events are identified in the three cities. Wind roses reveal statistical patterns during these pollution events with dominant northeast/southwest directions in Paris and Mexico City, and the transboundary transport of pollutants from the United States in Toronto. To check how well chemistry transport models perform during pollution events, we evaluate simulations made using the GEOS-Chem model for March 2011. In these simulations we find that NH3 concentrations are underestimated overall, though day-to-day variability is well represented. PM2.5 is generally underestimated over Paris and Mexico City, but overestimated over Toronto.