Optimizing the industrial structure of the Yangtze River Delta is the key to solving the structural contradictions of regional economic development. Based on the dynamic changes of the rationalization and heightening of the industrial structure, this paper selects the Theil index and the proportion of industry added value to quantify the aforementioned concept. According to the relevant data of the Yangtze River Delta industry in recent years, a regression analysis of the factors affecting the optimization of the regional industrial structure is carried out. The results are as follows: GDP per capita, fixed asset investment rate, and the process of urbanization all give impetus to the rationalization of the industrial structure. Emphasizing the role of supply and the balance of investment structure is the focus of policy decisions. The process of urbanization and marketization promotes the development of advanced industrial structure, which require government to promote the development of urban‐rural integration and minimize market intervention. Based on the analysis results, the Yangtze River Delta region should actively promote supply‐side structural reforms, attach importance to demand income elasticity and productivity enhancement benchmarks, achieve urban and rural integrated development, push forward industrial integration development, and play the decisive role of market allocation of resources to promote the progression of high‐quality economic development in the Yangtze River Delta region.