The removal of carbon dioxide from the atmosphere and its long-term storage in natural systems represents a critical ecosystem service (ES) in the context of climate change mitigation. This process, referred to as carbon sequestration, consists of the removal of carbon by vegetation and its storage in reservoirs, termed “carbon sinks”, such as soils, rocks, and water bodies. Despite their importance, the complex interactions between carbon sequestration and other ESs remain under investigated, especially in urban areas, where urbanization-driven land cover changes, usually resulting in land take and soil sealing, lead to a reduction in vegetated areas capable of removing and storing atmospheric carbon. This study presents an integrated methodological framework that combines a spatially explicit assessment of ESs with inferential modeling to explore the interdependence between carbon sequestration and other four ESs: regulation of local temperatures, regulation of pluvial runoff, habitat quality, and opportunities for nature-based recreation. Applied to the Functional Urban Area of Cagliari (Italy), the approach reveals a robust and positive association between carbon sequestration and the three regulating ESs. In contrast, a weak and inverse relationship with the availability of green areas as potential suppliers of nature-based recreational opportunities is highlighted. These results offer valuable insights for urban planning, thus demonstrating the utility of the proposed framework in supporting evidence-based decision-making.