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Land-use change is supposed to exert significant effects on the spatio-temporal patterns of ecosystem carbon storage in arid regions, while the relative size of land-use change effect under future environmental change conditions is still less quantified. In this study, we combined a land-use change dataset with a satellite-based high-resolution biomass and soil organic carbon dataset to determine the role of land-use change in affecting ecosystem carbon storage from 1980 to 2050 in the Gansu province of China, using the MCE-CA-Markov and InVEST models. In addition, to quantify the relative size of the land-use change effect in comparison with other environmental drivers, we also considered the effects of climate change, CO2 enrichment, and cropland and forest managements in the models. The results show that the ecosystem carbon storage in the Gansu province increased by 208.9 ± 99.85 Tg C from 1980 to 2020, 12.87% of which was caused by land-use change, and the rest was caused by climate change, CO2 enrichment, and ecosystem managements. The land-use change-induced carbon sequestration was mainly associated with the land-use category conversion from farmland to grassland as well as from saline land and desert to farmland, driven by the grain-for-green projects in the Loess Plateau and oasis cultivation in the Hexi Corridor. Furthermore, it was projected that ecosystem carbon storage in the Gansu province from 2020 to 2050 will change from −14.69 ± 12.28 Tg C to 57.83 ± 53.42 Tg C (from 105.62 ± 51.83 Tg C to 177.03 ± 94.1 Tg C) for the natural development (ecological protection) scenario. By contrast, the land-use change was supposed to individually increase the carbon storage by 56.46 ± 9.82 (165.84 ± 40.06 Tg C) under the natural development (ecological protection) scenario, respectively. Our results highlight the importance of ecological protection and restoration in enhancing ecosystem carbon storage for arid regions, especially under future climate change conditions.