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Whether the new type of urbanization implemented in China in the past decade has been effective in regulating urbanization and balancing human development and environmental protection remains to be verified. Therefore, this study develops a framework for assessing population-urbanization–ecological environment interactions by combining the coupling coordination degree model and the decoupling index. Firstly, the proposed framework establishes an indicator system of population, economy, society, space, environmental pressure, ecological governance, ecological status, and ecological services based on two sets of national census data; secondly, this study combines the coupling coordination degree model and decoupling index to comprehensively understand the coupling coordination relationship and the decoupling relationship of the population–urbanization–ecological environment across time and space. Overall, this study contributes to a deepened understanding of coupled population–urbanization–ecological environment interactions and provides a scientific basis for effective guidance on urban–rural management and the balance between human development and environmental protection.