Studies on land use structural optimization can support the sustainability of land resources. The Taipusi Banner lies in the arid and semiarid area of northern China, with rapid economic development and a vulnerable ecological condition. Taking the Taipusi Banner as a research case, we adopted a land use map and statistical data, and employed the ecosystem process model to establish five scenarios, including an economically optimal scenario, an ecologically optimal scenario, a comprehensively optimal scenario, a status quo, and a projected scenario. Based on multi-objective linear programming, the land use demand was optimized; then, the CLUE-S model and adaptability evaluation were adopted to establish spatial patterns. The ecological and economic benefits were then analyzed and policy suggestions are provided. The main results include the following: (1) The optimization outputs of various scenarios show that under optimization, cropland and forestland increased by 9.13% and 18.9%, respectively, and grassland decreased by 9.81%. (2) The land use optimization shows that comprehensive optimization aimed at achieving comprehensive benefits, ecological benefits, and economic benefits increased these benefits by 3.89%, 2.1%, and 6.2%, respectively. Compared with other scenarios, focusing on the comprehensive benefits of land use can result in the greatest increase in benefits to improve sustainability land resources. Land use optimization must consider not only the optimization of both the quantity and configuration but also the dimensions of both ecology and the economy. Land use should be based on a land suitability evaluation and optimization of the land use spatial configuration to update ineffective land uses and should gradually adjust both the ecological and engineering measures.
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