By using the methods of scenario analysis, model simulation, and the multi-objective spatial optimisation algorithm Non-dominated Sorting Genetic Algorithm-II (NSGA-II), the Pareto optimal solutions for water supply, water purification (N retention), as well as carbon storage and sequestration service (carbon service) of the Central Plains Urban Agglomeration (CPUA) were sought by adjusting the land use structure. It showed that, to reach the Pareto optimal solution goal, (1) in Scenario 1 (S1), the water supply service needs to increase by 10.682 billion cubic metres, the water purification (N retention) service needs to decrease by 11,400 tons, and the carbon service need to decrease by 2.487 billion tons. In Scenario 2 (S2), the water supply service needs to increase by 8.243 billion cubic metres, the water purification (N retention) service needs to decrease by 11,000 tons, and the carbon service needs to decrease by 2.466 billion tons. In Scenario 3 (S3), the water supply service needs to increase by 4.089 billion cubic metres, the water purification (N retention) service needs to decrease by 10,800 tons, and the carbon service needs to decrease by 2.380 billion tons. (2) After land use optimisation and adjustment, the S3 ecological land structure is complete and consistent with the vision of ecological protection and urban development in the study area, which is the optimal scenario. (3) Optimising the ecosystem service supply pattern through land use structure adjustment could balance the overall ecosystem service supply pattern of the study area In regions wherein ecosystem supply is insufficient and there is a spatial mismatch between supply and demand for ecosystem services, this study can guide regional land planning and assist in the formulation of ecosystem service management policies.