Land-use and land-cover changes (LUCCs) significantly impact carbon sequestration by modifying the structure and function of terrestrial ecosystems. This study utilized GIS and remote sensing techniques to forecast future LUCC patterns and their influence on regional carbon budgets, which is essential for sustainable development. We devised a coupled system dynamics (SD) model integrated with a patch-generating land-use simulation (PLUS) model to simulate LUCCs under diverse future scenarios using multisource environmental data. Additionally, the InVEST model was employed to quantify carbon storage in terrestrial ecosystems. By establishing three scenarios—ecological priority (EP), highly urbanized (HU), and coordinated development (CD)—this study’s aim was to predict the LUCC patterns and carbon storage distribution of the Tuojiang River Basin (TRB), China, up to 2035. The results showed that (1) from 2000 to 2020, significant LUCCs occurred in the TRB, primarily involving the conversion of cultivated land into construction areas and forestland; (2) LUCCs had a substantial impact on carbon storage in the TRB, with the EP scenario demonstrating the highest carbon storage by 2035 due to extensive forest expansion, while the HU scenario indicated a decline in carbon storage associated with rapid urbanization; and (3) the mountainous regions of the TRB, dominated by forestland, consistently exhibited higher carbon storage, whereas the Chengdu Plain region in the upper basin displayed the lowest. In conclusion, we recommend prioritizing the CD scenario in future development strategies to balance economic growth with ecological protection while simultaneously enhancing carbon storage. Our findings offer valuable insights to shape future LUCC policies in the Tuojiang River Basin, underscoring the adaptability of the coupled model approach to a wide range of geographic scales and contexts.