Against the intertwined strategic backdrop of China’s “dual carbon” initiative and high-quality urbanization drive, this paper systematically investigates the coupling coordination relationship and evolutionary trends between urbanization development and carbon emission efficiency across the 11 provincial-level administrative regions of the Yangtze River Economic Belt (YREB). Based on a constructed multi-dimensional comprehensive evaluation index system for urbanization and carbon emission systems, three mainstream econometric and simulation methods are adopted, including the entropy weight method, coupling coordination degree model, and system dynamics model to empirically examine the spatiotemporal evolution characteristics of urbanization-carbon emission coupling coordination during the period 2000–2021 and further predict its dynamic development trajectories for 2022–2032. The empirical results indicate that, first, the overall urbanization level of the YREB presents a fluctuating upward trend over the study period, with spatial urbanization serving as the core driving pillar. Meanwhile, the comprehensive carbon emission index increases steadily with pronounced and persistent regional heterogeneity across the region. Second, the regional coupling coordination degree demonstrates a continuous improving trend, while the developmental gaps among the eastern, central, and western sub-regions gradually diminish over time; Shanghai consistently maintains a pioneering level of coupling coordination throughout the whole period. Third, the upward evolution of coupling coordination is projected to sustain from 2022 to 2032. By 2032, all provincial-level regions in the YREB will achieve notable progress in coordinated development, with the majority entering the stage of good or superior coordination. On this basis, this study puts forward targeted policy implications for accelerating the low-carbon transformation of urbanization and promoting balanced and coordinated regional development in the YREB, which provides practical references for advancing the region’s sustainable transition and facilitating the realization of national “dual carbon” goals.