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Managing multiple ecosystem services (ESs) to facilitate synergy benefits is a crucial but challenging task for sustainable development, especially in arid and semi-arid regions. In this paper, the Inner Mongolia was used as a case study to systematically analyze the spatial trade-offs and synergies between 12 ESs consisting of 88 counties using the framework of ecosystem service bundle. We mapped ES distribution and then analyzed the relationships between ESs using Spearman correlation and hotspot/coldspot overlay analysis. In addition, ES bundles were identified using a self-organizing mapping network and the socio-ecological variables that drive the different ESs were explored using redundancy analysis. The results revealed complex spatial interactions between various ESs in Inner Mongolia due to water limitations. ES distribution and ES relationships correlated with gradients in biophysical and socioeconomic factors such as slope, precipitation, temperature, soil properties, and population density, and formed five types of ES bundles. These findings not only promote a clear understanding of the complex relationships among regional ESs, but lay a foundation for exploring win-win management strategies of ecological conservation and social-economic development in arid and semi-arid regions. • 12 ecosystem services were assessed at the county scale in Inner Mongolia. • Complex spatial interactions occurred between pairwise ecosystem services. • Self-organizing map method identified five types of ecosystem service bundles. [ABSTRACT FROM AUTHOR]