A GIS-based multicriteria decision analysis (MCDA) is presented to evaluate the suitability of land for the implementation of nature-based solutions (NbS) to enhance carbon sequestration in Emilia-Romagna, Italy. Excessive carbon emissions into the atmosphere have caused rapid and profound climate change that needs to be mitigated. The use of NbS has emerged as an effective strategy to sequester atmospheric carbon and improve environmental resilience. This study focuses on identifying the best NbS to maximise carbon sequestration for three environmental zones: urban, peri-urban and agricultural. The analysis identifies optimal locations for three area-specific NbS: street trees, green spaces and buffer strips. The region was divided into 30 × 30 m grid pixels, with each grid cell assigned a value from 1 (least suitable) to 5 (most suitable). The results show that most of the high-quality pixels are located near the main urban centres and along the coastline. These results provide useful information for policy makers and urban planners who can be guided in the strategic implementation of NbS to achieve maximum environmental benefits. The work also includes an individual sensitivity analysis to validate the robustness of the proposed model and a quantitative estimate of the carbon that can be sequestered by these NbS.