The Grain for Green Project (GGP) is one of many Nature-based Solutions (NbS), which aims to address the challenge of ecological restoration while providing livelihood security for farmers in poverty-dominated regions. Evaluating the success of such a project can prove difficult. Here, we choose the contiguous poverty-stricken regions (CPSR) of China to study the multiple benefits of the GGP in the context of NbS. We collect ecological-monitoring data, forest-resources data, and socioeconomic data and use them in a distributed method with relevant indicators, to evaluate the ecological benefits of the GGP. Additionally, the socioeconomic benefits are evaluated using questionnaire-based surveys. Our results showed that the ecological benefits of the GGP in the CPSR were 5.6 × 1011 RMB/a in 2017, with the proportion of each ecosystem’s services being 27.1% (water conservation), 21.1% (biodiversity conservation), 18.4% (purification of the atmospheric environment), 13.1% (soil conservation), 12.9% (carbon sequestration and oxygen release), 5.4% (forest protection), and 1.6% (nutrient accumulation). In terms of socioeconomic benefit, the GGP changed the production methods of farmers, which resulted in income growth, with an average increase of 5100 RMB/a per household. In the context of NbS, ecological conservation, and restoration, the accurate and systematic monitoring of the socioeconomic and ecological benefits will become more important for government decisions.