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Using the CRITIC method, comprehensive index evaluation method, VAR model, coupling coordination model and other methods, this paper evaluates the comprehensive development of the population economy and eco-geological environment composite system in the twin-city economic circle of Chengdu–Chongqing region from 2000 to 2020, verifies the dynamic coupling relationship between subsystems and measures the coupling coordination degree of complex system. Meanwhile, the differences in the development process of each subsystem are discussed and the spatial–temporal evolution characteristics and laws of coupling coordination of the composite system during the research period are analyzed. The results reveal the following: (1) There is a long-term coordinated relationship between population, economy and eco-geological environment in Chengdu–Chongqing region, which have the conditions for emergence and generation. (2) The subsystems of population, economy and eco-geological environment in Chengdu–Chongqing region show an overall upward trend, among which the Sichuan part obviously outperforms the Chongqing part. Besides, the growth rate of the economy subsystem is significantly higher than that of the population, eco-geological environment subsystem. (3) The coupling coordinated development of the composite system has shown a benign upward development trend, gradually changing from "composite spiral structure" to "two cores outstanding, peripheral collapse, the west superior to the east", while the main coordination state has developed from "Basic synergy—Economic lag" in 2000 to "Basic synergy—Population lag" in 2022. In addition, Cheng-De-Mian and Yuzhong districts with the better level of economic development have shown "Advanced synergy—Ecological lag". [ABSTRACT FROM AUTHOR]