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Planting green manure is an effective way to improve the agricultural environment and the quality of cultivated land in China. However, deviation from green manure planting willingness and behavior (DWB) becomes a serious obstacle to the promotion of green manure planting technology. For economic farmers, whether to plant green manure is a rational choice made after weighing up family endowments. In addition, ecological cognition plays a moderating role in the “willingness-behavior” transformation process of farmers’ green manure planting on the basis of family endowments. We selected four counties in which to conduct a questionnaire survey in Gansu and carried out interviews with 375 farmers. Based on the survey data, our study identified determinants that influence farmers’ DWB and examined the moderating effect of ecological cognition. In our paper, results show that the probability of farmers’ DWB is 41.87%. Farmers’ DWB is not only negatively affected by social network information and ecological compensation (eco-compensation) and positively influenced by the scale of cultivated land, but also restricted by human capital endowment characteristics such as age and education. In addition, ecological cognition played a significant moderating effect on farmers’ DWB. Farmers with high ecological cognition were more aware and capable of promoting green manure planting intentions into practice. Furthermore, different groups of farmers had different characteristics of DWB. The findings are useful and helpful in better understand the influencing factors of farmers’ DWB for policy makers and managers and can provide some effective support for policies designed to encourage farmers to adopt more sustainable green manure.