Within the sustainable urbanization framework, two dimensions, namely, social urbanization and environmental urbanization, have complex coordinated interactions. To better understand the coordinated interaction status between the two dimensions of sustainable urbanization, an empirical study was carried out in the 14 cities of Hunan Province, China, from 2011 to 2019. This study establishes an integrated measurement framework, uses the coupling coordination degree model, information entropy weight analysis approach, and the Technique for Order Preference by Similarity to an Ideal Solution method to analyze the development degrees and coordinated interaction degrees of the two dimensions. The results show that the quality and efficiency of leisure facilities and water use have the greatest impacts on the coordinated interactions between the two dimensions. Besides, the development degrees of social urbanization and environmental urbanization are not consistent. What is more, the spatial noncorrelation of the coordinated interaction status demonstrates that the “high-quality development” tactics aiming to promote balanced development of dimensions among cities in China is feasible. Furthermore, corresponding suggestions are proposed, providing references for governments’ planning and decision-making processes.