With the advancement of urbanization and industrialization, the territorial spatial structure of urban-marginal-rural regions has undergone significant changes, which have profound impacts on land use patterns as well as a complex effect on Ecosystem Services (ESs) and their trade-offs and synergies. Under the context of urban-rural integration and high-quality development, systematically analyzed the dynamic evolution of the territorial spatial structure of urban-marginal-rural regions, and explored the influence mechanism of land use changes on ESs trade-offs and synergies, and then proposed optimization strategies, are of great academic significance and practical value for rationally optimizing the allocation of land resources, improving ESs, and promoting sustainability. This study, taking Suzhou as an example, identified its urban-marginal-rural territorial spatial structure for the years 2005 and 2022 based on multi-source data using Deep Neural Network (DNN) and semi-supervised learning methods. The InVEST model was employed to evaluated the four major ESs, namely, water yield, carbon storage, habitat quality, and soil retention. After determining the correlation between groups of ESs using the Pearson correlation coefficient, the Ecosystem Services Trade-off Degree (ESTD) model was used to determined the relationship between the trade-off degree of each group of ESs. A Hierarchical Linear Model was used to investigated the process of the geographical and temporal development of land use, taking into consideration the spatial structure of the urban-marginal-rural area and the synergistic trade-offs of the ESs. Conclusions are drawn: (1) From 2005 to 2022, the territorial spatial structure of urban-marginal-rural regions in Suzhou underwent considerable changes, with 79.29% of rural areas evolving into marginal zones and 99.48% of marginal zones transformed into urban areas. (2) Based on the dynamic evolution of the urban-marginal-rural territorial spatial structure, the study analyzed the trade-off synergistic relationship of ESs in five types of territories: urban maintenance area, urban expansion area, marginal area maintenance area, marginal area expansion area, and rural retention area. In the marginal area expansion area and the urban expansion area, it showed a significant trade-off relationship, while in the marginal area maintenance area and the urban maintenance area, it showed a coexisting relationship of trade-off synergistic relationship. (3) The spatiotemporal evolution of land use, taking into account the spatial structure of the urban-marginal-rural area, had a significant negative effect on the synergy of trade-offs of ESs, and the negative effect was more prominent in the three regions of the urban expansion area, the persistent marginal zone, and the marginal zone expansion area, particularly in the persistent marginal zone and the marginal zone expansion area. (4) Given the characteristics of urban-marginal-rural area human-land relations, this study proposed strategies for optimizing land use in each region under the synergistic objectives of ESs, such as optimized the spatial layout of the city, promoted the ecological agricultural model, controlled the region's expansion rate, established ecological corridors and buffer zones, and carried out multifunctional land use planning.