Rural livelihoods, which are basic human activities, have long interacted with the environment. In light of the complexity of the human–environment system, more interdisciplinary analyses from geographical, environmental, and social sciences are needed. Using qualitative and quantitative methods from social, environmental, and geographical sciences, this study conducted a geographical regionalization and a comparative analysis of rural livelihoods in different zones in the Loess Plateau to explore the relationship between rural livelihoods and the environment. The results indicated that rural livelihoods are tightly coupled with the environment on a village scale, showing significant geographical regularity and spatial disparity. A combination of geographical location, resource endowment, and environmental sanitation affects rural livelihoods in terms of spatial patterns, development capacity, and quality of life in the context of the public ownership system, the utilization policy of land resources, and limited technical conditions. Coupling the relationship between rural livelihoods and a given environment on a village scale tends to lead to one of four types of relationships: “homeostatic”, “intense”, “transferred”, or “optimized”. Accordingly, governments and policymakers need to consider that countryside revitalization must be locally tailored and implemented through the four aspects of “rights revitalization”, “labor revitalization”, “industrial revitalization”, and “environmental revitalization”.