This paper optimises projected land-use structure in 2020 with the goal of increasing terrestrial ecosystem carbon storage and simulates its spatial distribution using the CLUE-S model. We found the following: The total carbon densities of different land use types were woodland > water area > cultivated land > built-up land > grassland > shallows. Under the optimised land-use structure projected for 2020, coastal Jiangsu showed the potential to increase carbon storage, and our method was effective even when only considering vegetation carbon storage. The total area will increase by reclamation and the original shallows will be exploited, which will greatly increase carbon storage. For built-up land, rural land consolidation caused the second-largest carbon storage increase, which might contribute the most as the rural population will continue to decrease in the future, while the decrease of cultivated land will contribute the most to carbon loss. The area near the coastline has the greatest possibility for land-use change and is where land management should be especially strengthened.