The Chinese government has implemented a series of ecological restoration projects in the Loess Plateau (LP), and the surface cover changed dramatically, impacting the ecosystem services (ESs) greatly. In this study, we used K-means clustering to classify the land use structures (LUSs) of the LP from 1990 to 2015 at the small watershed scale, and investigated the effects of LUS on water supply (WS), soil conservation (SC), and carbon sequestration (CS, expressed as NPP) with constraint lines. The values of WS and SC were obtained from the InVEST simulation, validated by the hydrographic station data. The results showed that the LUSs in LP were cropland structure (CLS, distinguished with CS), forest structure (FS), grassland structure (GS), crop-grassland structure (CGS), crop-forest-grassland structure (CFGS) and a very few areas of barren structure (BS). The proportion of dominant land use in those LUSs with a balance of WS, SC, and CS was 0.6–0.7 (cropland in CLS), 0.5 (forest in FS), 0.45/0.4 (cropland/grassland in CGS), 0.75 to 0.85 (grassland in GS), and 0.15/0.4/0.25 to 0.35 (cropland/forest/grassland in CFGS), respectively. The types of constraint curves of ESs for those LUSs involves hump-shaped curve, negative convex, half-concave-waved curve and concave-waved curve. This study proposed a method to objectively delineate LUS and improved the constraint line method to make it suitable for cases with less data, innovatively presenting the variation of ESs inside LUSs, which may provide a reference for optimal land planning and sustainable development of social-ecological systems.
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