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Liaoning Province, as an old industrial urban agglomeration since the founding of China, is an important link between the Bohai Economic Zone and the Northeast Economic Zone, and it has made great contributions to the economic development of China. The transformation of China’s economy and heavy industrial development have posed great challenges to the long-lasting growth of Liaoning Province. In this study, the driving force of land expansion was detected using the patch-generating land use simulation (PLUS) model in Liaoning Province, and the land situation in 2030 was predicted under natural development, ecological protection, and economic development scenarios. We then further coupled the PLUS model with the integrated valuation of ecosystem services and trade-offs (InVEST) model to explore the spatial autocorrelation and synergistic relationship between carbon storage and habitat quality. The results indicated the following: (1) The total accuracy of the simulation in 2020 using the PLUS model reached 94.16%, and the Kappa coefficient reached 0.9089; therefore, the simulation result was highly reliable. (2) The overall spatial pattern of both carbon storage and habitat quality decreased from the northwest and southeast to the middle, and habitat quality had an impact on carbon storage to a certain extent, with a positive spatial correlation. (3) The ecological protection (EP) scenario was the only development prospect with increasing total carbon storage, which could increase carbon sequestration by approximately 7.83 × 106 Mg/C, and development prospects with optimal habitat quality. (4) Weak trade-off and weak synergy dominated in the 2030 natural development (ND) scenario; most regions showed weak synergy in the ecological protection scenario, spatial heterogeneity became more pronounced in the economic development (ED) scenario, and a strong trade-off and strong synergy emerged in individual regions. The results of the study have a positive feedback effect on establishing an ecological security barrier in Liaoning Province and furthering long-lasting low-carbon urban development.

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