Mounting research highlights the contribution of ecosystem services provided by urban forests to quality of life in cities, yet these services are rarely explicitly considered in environmental policy targets. We quantify regulating services provided by urban forests and evaluate their contribution to comply with policy targets of air quality and climate change mitigation in the municipality of Barcelona, Spain. We apply the i-Tree Eco model to quantify in biophysical and monetary terms the ecosystem services “air purification,” “global climate regulation,” and the ecosystem disservice “air pollution” associated with biogenic emissions. Our results show that the contribution of urban forests regulating services to abate pollution is substantial in absolute terms, yet modest when compared to overall city levels of air pollution and GHG emissions. We conclude that in order to be effective, green infrastructure-based efforts to offset urban pollution at the municipal level have to be coordinated with territorial policies at broader spatial scales.