Poverty and environmental degradation is an interactive and complex issue, which needs to be addressed to pursue human sustainable development. The objective of this study was to create a theoretical framework for sustainable agriculture, considering the dynamic interaction between environment and multidimensional poverty. The model system used in this study was the region surrounding the Chinese Three Gorges reservoir. We constructed an evaluation index system to measure the dynamic interactions by employing Entropy-weight and analytic hierarchy process (AHP) methods. In this case study, we analyzed the dynamic interactive relationships between environmental degradation and rural poverty by adopting geographic information system (GIS) and comprehensive index evaluation, based on statistical (2000–2013) and remote sensing image data. We found that: (i) in the Three Gorges reservoir region (TGRR), a vicious cycle between poverty, environmental load, and livelihood is occurring; (ii) in areas stressed by environmental concerns the environmental load is the main stress factor, while in the areas stressed by poverty, livelihood is the main stress factor; and (iii) the coupling degrees between environmental degradation and poverty differ in different areas of the TGRR, and counties with adverse features have been spatially agglomerated over time; and the area with high coupling and high synergy accounts for the 38.1% of the total reservoir region.