This study aims to scientifically justify the identification of suitable urban properties for urban green infrastructure (UGI) interventions to optimize its natural regulating functions for long-term pollution mitigation and secondary dust reduction. This study adheres to the perception that planning urban transformations to improve ambient air quality (AQ) requires a thorough understanding of urban structural heterogeneity and its interrelationship with the local microclimate. We apply an approach in which UGI and its potential multifunctionality are explored as a structural–functional element of urban local climatic zones. The same (100 × 100 m) spatial framework is used to develop place-based adapted solutions for intervention in UGI. A complex geospatial analysis of Burgas City, the second largest city (by area) in Bulgaria, was conducted by integrating 12 indicators to reveal the spatial disbalance of AQ regulation’ demand and UGI’s potential to supply ecosystem services. A total of 174 municipally owned properties have been identified, of which 79 are of priority importance, including for transport landscaping, inner-quarter spaces, and social infrastructure. Indicators of population density and location of social facilities were applied with the highest weight in the process of prioritizing sites. The study relies on public data and information from the integrated city platform of Burgas, in cooperation with the city’s government. The results have been discussed with stakeholders and implemented by the Municipality of Burgas in immediate greening measures in support of an ongoing program for Burgas Municipality AQ improvement.