Air pollution has been a major threat to human health, ecosystems, and agricultural crops ever since the onset of widespread use of fossil fuel combustion and emissions of harmful substances into ambient air. As a basis for the development, implementation, and compliance assessment of air pollution control policies, monitoring networks for priority air pollutants were established, primarily for regulatory purposes. With increasing understanding of emission sources and the release and environmental fate of chemicals and toxic substances into ambient air, as well as atmospheric transport and chemical conversion processes, increasingly complex air pollution models have entered the scene. Today, highly accurate equipment is available to measure trace gases and aerosols in the atmosphere. In addition, sophisticated atmospheric chemistry transport models—which are routinely compared to and validated and assessed against measurements—are used to model dispersion and chemical processes affecting the composition of the atmosphere, and the resulting ambient concentrations of harmful pollutants. The models also provide methods to quantify the deposition of pollutants, such as acidifying and eutrophying substances, in vegetation, soils, and freshwater ecosystems. This article provides a general overview of the underlying concepts and key features of monitoring and modeling systems for outdoor air pollution.