Persistent Organic Pollutants (POPs) are global pollutants that can migrate over long distances and bioaccumulate through food webs, posing health risks to wildlife and humans. Multilateral environmental agreements, such as the Stockholm Convention on POPs, were enacted to identify POPs and establish the conditions to control their release, production and use. A Global Monitoring Plan was initiated under the Stockholm Convention calling for POP monitoring in air as a core medium; however long temporal trends (>10 years) of atmospheric POPs are only available at a few selected sites. Spatial coverage of air monitoring for POPs has recently significantly improved with the introduction and advancement of passive air samplers. Here, we review the status of air monitoring and modeling activities and note major uncertainties in data comparability, deficiencies of air monitoring and modeling in urban and alpine areas, and lack of emission inventories for most POPs. A vision for an internationally-integrated strategic monitoring plan is proposed which could provide consistent and comparable monitoring data for POPs supported and supplemented by global and regional transport models. Key recommendations include developing expertise in all aspects of air monitoring to ensure data comparability and consistency; partnering with existing air quality and meteorological networks to leverage synergies; facilitating data sharing with international data archives; and expanding spatial coverage with passive air samplers. Enhancing research on the stability of particle-bound chemicals is needed to assess exposure and deposition in urban areas, and to elucidate long-range transport. Conducting targeted measurement campaigns in specific source areas would enhance regional models which can be extrapolated to similar regions to estimate emissions. Ultimately, reverse-modeling combined with air measurements can be used to derive “emission” as an indicator to assess environmental performance with respect to POPs on the country, region, or global level.