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Assessing the impacts and drivers of urban expansion on terrestrial carbon storage (TCS) is important for urban ecology and sustainability; however, a unified accounting standard for carbon intensity and research on the drivers and economic value of TCS changes are lacking. Here, urban expansion and TCS in the Yangtze River Delta were simulated based on Patch-generating Land Use Simulation and Integrated Valuation of Ecosystem Services and Trade-offs models; scenario simulation; Literature, Correction, Ratio, Verification carbon intensity measurement; and land use transfer matrix methods. The results showed that (1) from 2000 to 2020, urbanization and TCS loss accelerated, with 61.127% of TCS loss occurring in soil, and land conversion was prominent in riverine and coastal cities, mainly driven by the urban land occupation of cropland around suitable slopes, transportation arteries, and rivers. (2) From 2020 to 2030, urban land expansion and TCS loss varied under different scenarios; economic losses from the loss of the carbon sink value under cropland protection and ecological protection were USD 102.368 and 287.266 million lower, respectively, than under the baseline scenario. Even if urban expansion slows, the loss of TCS under global warming cannot be ignored. Considering the indirect impacts of urbanization, the failure to establish a regional development master plan based on ecosystem services may affect China’s carbon targets.
