This paper firstly proposed an analytical framework for the relationship between ecosystem services value (ESV) and multidimensional poverty-reduction index; then, it conducted a quantitative assessment of ESV including ecosystem disservices in China’s Three Gorges Reservoir region; next, it explored the interactive relationship between ESV and multidimensional poverty-reduction index in an attempt to reveal the contribution of ecosystem services to poverty reduction in this special region. The results indicate that: (1) There is a long-term co-integration between ESV and multidimensional poverty-reduction index, and their coupling degree is on the rise; ESV plays an important role in improving social security and mitigating poverty; (2) There are high correlations between climate regulation, waste treatment, maintenance of genetic diversity, environment purification, landscape aesthetics, maintenance of soil fertility and multidimensional poverty-reduction index, making the greatest contribution to poverty reduction in the region; and (3) Contributions of different specific ecosystem services to poverty reduction are varied considerably among different categories of ESV. Finally, this paper proposed policy recommendations for the synergy between eco-environmental protection and poverty reduction based on the findings of this research.