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Energy consumption and environmental pollution are along with urban sprawling, while the impact of urbanization on energy and environment is quite controversial. The study of urbanization and energy-environmental efficiency provides a new perspective to understand the correlation between urbanization, energy consumption and environment. In this paper, a Directional Distance Function-Data Envelopment Analysis (DDF-DEA) model is employed to investigate provincial energy-environment efficiency in China from 1999 to 2017. Then the mechanism of urbanization substantially affecting the energy-environment efficiency is empirically examined from the perspective of government and market, respectively. The results indicate that China’s energy-environmental efficiency is improving, but regional differences exist and have widened since 2005; the overall impact of urbanization on China’s energy-environment efficiency is negative while the mechanism differs between different regions. Specifically, government-dominated urbanization has promoted energy-environment efficiency in the eastern region, while has a negative impact in the central and western regions; market-led urbanization has a limited positive impact on energy-environment efficiency. These conclusions proved to be robust, and are of great significance for policymakers to take full use of the positive externality of urbanization to promote the energy-environment efficiency and improve the environment.