This paper explores the coupling relationship between land use and rural development to improve the environmentally friendly level of land use and attain accelerated rural revitalization. On the basis of the coupling framework, the quantitative study included the dimensionless method, the entropy method, and the coupling measure model with an empirical study in the Hainan province of China. Specifically, we evaluated levels of environmental friendliness and rural revitalization, and further calculated the coupling degree, coupling coordination degree, and the relative development degree between the two. Results demonstrated that (1) both the levels of environmentally friendly land use and rural revitalization showed an upward trend; (2) the coupling degree between environmentally friendly land use and rural revitalization was always at a high level; (3) the coupling coordination degree was improved from reluctant coordination to a quality coordination level; and (4) the relative development degree has changed since 2014, and environmentally friendly land use began to lag behind rural revitalization. This study contributes to the literature by integrating the coupling model into the relationship between land use and rural development, and the results of the article can provide a reference for China and other developing countries to coordinate land use and rural development.