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According to the “dual-carbon” goal, the solution to achieving balanced regional development and industrial structural optimization while promoting sustainable development goals lies in the synergistic evolution mechanism of carbon emission efficiency and green technological innovation. Using provincial panel data from China from 2000 to 2022, this study calculates industrial structural optimization coefficients for the “advanced,” “rationalization,” and “ecology” dimensions. The impact of green technological innovation on industrial structural optimization is experimentally explored using panel regression, threshold effect, and mediating effect methodologies, based on the constraint perspective of carbon emission efficiency. The findings show that (1) the optimization of the regional industrial structure is successfully driven by both carbon emission efficiency and green technological innovation; (2) the impact of green technological innovation on industrial structural optimization is positively regulated by carbon emission efficiency, which also helps to achieve sustainable economic transformation; and (3) this moderating effect exhibits significant regional heterogeneity and U-shaped nonlinear characteristics, in the order of “central > west > east”. This study reveals how green technological innovation affects industrial structural optimization under the constraint of carbon emission efficiency. It offers reference recommendations for the creation of sustainable development policies in the future.
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