In considering regional sustainable development, optimizing the distribution of land use and land cover (LULC) and improving terrestrial ecosystem carbon storage (CS) have emerged as major concerns. In this study, considering the synergistic effect between LULC and CS, a coupling model (named MPI) that integrates Multi-objective Optimization (MOP) model, the Patch-generating Land Use Simulation (PLUS) model, and the Integrated Valuation of Ecosystem Services and Trade-offs (InVEST) model, was proposed to simulate the 2030 CS and explore its spatial-temporal characteristics in a Beijing-Tianjin-Hebei urban agglomeration (BTH). The MPI model, which combines the advantages of the above three models, can optimize the LULC structure, simulate the LULC distribution, and efficiently extract CS variation. The results indicated that: (1) LULC changes in BTH were mostly represented in transfers between cropland, forest, and grassland; (2) three different scenarios were simulated using the MPI model, named BAU (Business as usual), EDP (Ecological development priority), and EEB (Ecological and economic balanced). The simulation results of the three scenarios are in line with their respective goals, and the results are quite different; (3) cropland, water, and bare land, will be reduced, and the constant shrinking of water is a pressing issue that must be addressed; and (4) the EEB scenario balanced ecological services and economic rewards, increased the ecosystem carbon sink function, and is an efficient way to investigate “carbon neutrality”. The application of the MPI model is of reference value for exploring the optimal configuration of land resources.