Abstract: Taking advantage of the opportunity for non-point source pollution control in the Chitian Reservoir watershed, we aimed to establish a green industrial model combining mango (Mangifera indica)||tiger milk mushroom (Lignosus rhinocerotis) production. This model has significant development potential as a pollution control resource and for economic growth. However, at present, the economic and ecological benefits of the “mango||tiger milk mushroom” model have not been quantified, which hinders the provision of effective data on pollution control of mango orchards and income increase of orchard farmers in the Chitian Reservoir basin. This study presents a comprehensive life cycle assessment and economic analysis method to compare the environmental and economic benefits of mango monoculture and mango||tiger milk mushroom intercropping systems. The life cycle assessment results indicated that the mango||tiger milk mushroom intercropping system had higher potential environmental impacts, especially in the category of climate change, freshwater ecotoxicity, and land use, which were 17.19, 11.44, and 19.57 times, respectively, of those of the mango monoculture system. This is mainly owing to the significant environmental effects caused by inputs, such as mushroom spawn sticks and transportation. To better compare the environmental impacts of the mango monoculture and mango||tiger milk mushroom intercropping systems in the field, the inputs of mushroom spawn stick and transportation were excluded, the results showed that the potential environmental impacts of the mango||tiger milk mushroom intercropping system were reduced by 58.91%−99.86% compared to those of the mango monoculture, except for the category of water consumption, which remained higher. In the mango monoculture system, farm emissions and fertilizers were the key factors contributing to the environmental load. Economic analysis revealed that the mango||tiger milk mushroom intercropping system had higher costs and revenues, which were 2.51 and 22.50 times, respectively, of those of the mango monocropping system. The main reason for this is that the mango||tiger milk mushroom system requires more material input, but the price of tiger milk mushroom is higher. The profit and cost-benefit ratios of the mango||tiger milk mushroom intercropping system were 41.64 and 16.60 times, respectively, higher than those of the mango monoculture system. These results suggest that the mango||tiger milk mushroom intercropping system is beneficial for reducing environmental impacts during field cultivation and increasing economic benefits. Governments should formulate appropriate incentive and promotion policies to encourage farmers’ willingness to adopt the “mango||tiger milk mushroom” cultivation model, thereby reducing environmental impacts, improving the ecological environment, and increasing farmers’ incomes.