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Low‐carbon sustainable development is considered an essential strategy for achieving economic growth and environmental protection, requiring a fundamental transformation of the industrial structure, including developing clean technologies, promoting energy efficiency, and adopting sustainable production and consumption patterns. Simultaneously, the evolving digital economy is acknowledged as an essential driver in optimizing the industrial structure. Therefore, can digital economy development reshape the industrial structure and lead to low‐carbon sustainable development? The main purpose of this paper is to examine the mediating role of industrial structure upgrading in the relationship between the digital economy and low‐carbon development. Its ultimate purpose is to explore more possible paths to achieve low‐carbon development. This paper builds a regression model based on the data of cities. We found that digital economic development can directly promote low‐carbon sustainable development, a conclusion that still holds after endogeneity discussion and robustness testing. Additionally, digital economy development can promote industrial structure upgrading and thus promote low‐carbon sustainable development, meaning that industrial structure upgrading is an effective mechanism for digital economy development to promote low‐carbon sustainable development. This paper provides empirical evidence for the positive environmental externalities of digital economic development and establishes a basic research framework of "digital economic development → industrial structure upgrading → low‐carbon sustainable development." [ABSTRACT FROM AUTHOR]