The interaction between rural household livelihood strategies and land use behavior constitutes the core of the human–land relationship in a region, especially in protected area villages with high ecological sensitivity that require the integration of social–economic and ecological benefits. This study, grounded in the concept of sustainable livelihoods, utilizes survey data from 399 households in the Chang-Zhu-Tan Green Heart Ecological Protection Zone. By employing the entropy method to calculate indicator weights, a coupling coordination degree model is constructed to analyze the coupling degree, coordination degree, and spatial differentiation patterns between household livelihood strategies and land use behavior. The findings reveal that (1) there is a coupling relationship between household livelihood strategies and land use behavior in the protected area, characterized by moderate coupling coordination. (2) Agricultural sideline households exhibit the highest degree of coupling coordination. The sideline activities of these households not only enhance income but also exert positive impacts on the ecological environment while they are engaged in agricultural production. (3) There is a significant spatial differentiation in the coupling coordination degree of different types of households in the protected area: it increases with the distance from the urban center, with higher values in the central areas than in the peripheral regions. The results of this study provide a basis for understanding micro-level land use changes and guiding household land use behavior, as well as offering theoretical and practical references for improving sustainable livelihoods of households in the study area, promoting rural revitalization, and implementing ecological protection policies.