Based on an analysis of related core papers and reports, this review presents a historical perspective on ambient air pollution and ambient air quality development in the modern-day Czech Republic (CR) over the past seven decades, i.e., from the 1950s to the present. It offers insights into major air pollution problems, reveals the main hot spots and problematic regions and indicates the principal air pollutants in the CR. Air pollution is not presented as a stand-alone problem, but in the wider context of air pollution impacts both on human health and the environment in the CR. The review is arranged into three main parts: (1) the time period until the Velvet Revolution of 1989, (2) the transition period of the 1990s and (3) the modern period after 2000. Obviously, a major improvement in ambient air quality has been achieved since the 1970s and 1980s, when air pollution in the former Czechoslovakia culminated. Nevertheless, new challenges including fine aerosol, benzo[a]pyrene and ground-level ozone, of which the limit values are still vastly exceeded, have emerged. Furthermore, in spite of a significant reduction in overall emissions, the atmospheric deposition of nitrogen, in particular, remains high in some regions.