Green innovation has become the mainstream of the era, and New Urbanization is an inevitable choice in the process of urbanization in China. Focusing on the topics of green innovation and new urbanization, much work has been done to find their factors respectively while the relationship between the two remains to be explored. Hence, in this article, representative indicators of new urbanization and green innovation are selected to study the Yangtze River Delta City Group from the perspective of both the entire urban agglomeration and a single city, in terms of time and space, using the entropy method and the coupling model. The results show that (1). Green innovation promotes the new urbanization development and there is a synergistic effect between the two systems. (2). The level of economic development is an important factor that affects the degree of coupling degree and coordination degree between the two interactions, and its influence is better than the spatial effect. (3). Green innovation and new urbanization have positive spatial autocorrelation and regional agglomeration (there are High-High, Low-Low, and High-Low collections).