Rapid urbanization has profoundly impacted regional ecosystem services. However, few studies have comprehensively examined the spatiotemporal relationship between multi-dimensional urbanization processes and ecosystem services. This study investigated the spatiotemporal dynamics of urbanization and ecosystem services value (ESV) in the Yangtze River Delta (YRD) region, China, from 2010 to 2020. We measured urbanization levels from two dimensions: Urbanization I (demographic, economic, and land urbanization) and Urbanization II (social and cultural urbanization). The ESV was quantified using the equivalent factor method. The results showed that: (1) The level of Urbanization I increased steadily, while Urbanization II, despite a lower level, exhibited a faster growth rate, especially after 2017; (2) The total ESV declined, with regulating services decreasing the most. The spatial distribution of ESV showed significant heterogeneity; (3) Urbanization had a significant negative correlation with ESV, with Urbanization I exerting a greater negative impact than Urbanization II; (4) The eastern region was dominated by high urbanization-low ESV clusters, while the western region was characterized by low urbanization-high ESV clusters. The findings provide important implications for regional sustainable development and can serve as a reference for related studies in other rapidly urbanizing areas around the world.