This study selects the data of 30 provinces in China (excluding Hong Kong, Macao, Taiwan, and Xizang) from 2011 to 2021 as a sample, and explains the mechanism of the role of environmental regulation on the high-quality development of the economy from direct and indirect aspects by constructing an index of high-quality development of the economy, and at the same time, analyzes the green technological innovation with the GTFP index measured by the super-efficiency SBMGML method as a proxy variable for the green technology innovation as a proxy variable to analyze the moderating effect of green technology innovation in the process of environmental regulation and economic high-quality development. The main conclusions are as follows: Environmental regulation can significantly promote high-quality economic development, and its promotion effect is still very obvious after combining it with the moderating variable of green technological innovation. There is a positive spatial spillover effect of environmental regulations in the process of promoting high-quality economic development. The main contribution of this paper is to enrich the research in the field of environmental regulation and high-quality economic development, which not only provides a theoretical and empirical basis for China’s future development, but also provides empirical support for developing countries.