The present study synthesizes the results of the complex field, laboratory and analytical research aimed at developing and evaluating technological and nature-based solutions for sustainable urban development, conducted in the town of Smolyan, Bulgaria. The main contributions cover scientific, applied, methodological and social aspects of the researched issues, providing a scientifically based methodology for selecting suitable locations for air pollution monitoring and assessment in the urban environment, as well as effective nature-based solutions to be implemented. Statistical evaluation confirmed the dependencies between the air quality and morphological characteristics of the urban topography, such as building density, presence of green areas and transport axes. The results from the biomonitoring revealed some correlations between the levels of air pollution and the content of potentially toxic elements in plant samples, reflecting the response of living organisms to adverse environmental conditions. Based on the metabolic changes found in the studied tree species, their suitability for landscaping areas with deteriorated air quality was assessed. Scientifically based recommendations were provided to support local policies on sustainable development and environmental planning. Cooperation between scientific institutions, municipal structures and civil society in the field of sustainable urban environment management was stimulated. Awareness of the benefits of nature-based solutions and their role in climate change adaptation was also increased.