Urbanization, as an important engine of modernization, plays an important role in promoting regional economy and improving living standards. Nevertheless, unchecked urban expansion over recent decades has strained natural resources and the environment, leading to crises, especially in densely populated urban areas that act as ecological barriers within river basins. The investigation of the interactive coercive relationship between the urbanization level (UL) and eco-environmental quality (EEQ) can facilitate the identification of sustainable pathways towards regional sustainability. Therefore, this study employed a set of multidisciplinary approaches, integrating simple linear regression, bivariate spatial autocorrelation, and coupling coordination degree (CCD) models, alongside multi-source remote sensing data to analyze the interactive coercive relationship between UL and EEQ in the Yangtze and Yellow River basins (YYRBs) in China. Key findings included a 6.97% improvement in EEQ in the Yellow River basin (YLRB) from 2001 to 2020, with higher values in the southeastern and southwestern regions and lower values in the central region, while the Yangtze River basin (YTRB) saw only a 1.28% increase, characterized by a lower EEQ in the west and higher levels in the middle and east, although the Yangtze River Delta showed a decline and significant variation among tributaries. UL rose steadily in both basins, especially in the middle reaches of the YLRB. Spatial autocorrelation analysis revealed a positive correlation between UL and EEQ in the YLRB, whereas a negative correlation was found in the YTRB. The CCD between UL and EEQ in the YYRBs improved, particularly in the middle and lower reaches, indicating the need for integrated urban development strategies that consider regional ecological capacities. These findings provided a scientific basis for ecological protection and sustainable urban development at a large river basin scale.