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Rapid urbanization improves socioeconomic development but challenges ecosystem sustainability. Meanwhile, the gradient responses of ecosystem services (ESs) to landscape structures and associated regime shifts of the agriculture–ecosystem–economy nexus (AEEN) have not been sufficiently addressed, preventing an effective balance between socioeconomic prosperity and ecosystem conservation. To bridge this knowledge gap, this study selected the Guangdong Province of southeastern China to explore landscape dynamics from 1985 to 2020 and their spatially heterogeneous impacts on ESs and the AEEN, based on Integrated Valuation of Ecosystem Services and Trade-offs approach and other biophysical models as well as statistical records about socioeconomic factors. AEEN elements, including ESs, responded directly to policy adjustments in terms of ecosystem restoration and landscape management and presented remarkable regime shifts (i.e., phase changes) and spatial heterogeneity. Aggressive agricultural reclamation before 1999 increased crop productivity but caused vegetation degradation and biomass decline. Accelerated urban expansion and ecosystem restoration efforts have improved economic and ecological benefits but have substantially reduced crop productivity and threatened food security. However, timely policy adjustments since 2009 reversed the declining trend and maintained the grain supply. Landscape composition presented patterns of gradual decline along the urban–rural gradient, which in turn determined ES gradient patterns. For instance, water yield and nitrogen export positively correlated with each other (p < 0.0001) but negatively correlated with other ESs. Our study enriches the understandings of social–ecological systems' response to man-made interventions from AEEN perspective allowing for spatial variabilities and regime shifts, which support policy formulation for coordinating ecological and economic benefits. [ABSTRACT FROM AUTHOR]