Exploring the spatiotemporal characteristics of ecosystem services (ESs) and their drivers is crucial for managers to develop significant scientific policies that further sustainable development. We used the Yangtze River Economic Belt (YREB) to explore the trends, hotspots, and drivers of water yield (WY), soil conservation (SC), carbon sequestration (CS), and food supply (FS) between 2000 and 2020. Similarly, we analyzed relationships among ESs and drivers of the multiple ecosystem services landscape index (MESLI). We used the self-organizing map method to obtain the types and distribution of the ES bundles, revealing the bundles, trade-offs, and synergies among ESs. The four ESs had an increasing trend, with CS having the highest increase; ES hotspot analysis showed differences among upper, middle, and lower reaches. Constraint lines among ESs and drivers were diverse; the corresponding SC and WY reached thresholds when CS values were 1477.81 and 460.5 t km−2, respectively. When FS values were 67.34 and 86.17 × 104 Yuan·km−2, CS and WY reached their thresholds. All critical drivers of the four ESs were natural factors. The thresholds that the MESLI reached with driver status were 1000 mm (evapotranspiration), 2121 mm (precipitation), 2.42° (slope), 1.46% (soil organic matter), 36.08% (sand), 30.75% (proportion of non-agricultural population), 18.57% (cropland proportion), 1.05 × 104 persons·km−2 (population density), and 84.84% (proportion of non-agricultural industries in total gross domestic product), respectively. FS, water supply, and ecological conservation bundles changed over the 20 years, and trade-offs and synergies among ESs within bundles differed. We revealed the complexity of ESs from multiple perspectives, which will enable the development of ecosystem management and conservation recommendations for the YREB and large-scale economic zones worldwide.
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