The effects of forest restoration on ecosystem services and their trade-offs are increasingly discussed by environmental managers and ecologists, but few demonstrations have analyzed ecosystem service trade-offs with a view to informing afforestation choices. Here, we examined how the Grain for Green Program (GGP), an ambitious reforestation program in China, affected ecosystem services. We quantified regulating services and provisioning service in the potential scenarios, which were developed to improve ecosystem services better. The results indicated the GGP drove 14.5% of land-use/land-cover from 2000 to 2015, and all the regulating services increased. Prioritizing reforestations in steep-sloped and riparian farmlands can promote flood mitigation, water purification, and soil retention services by 62.7%, 25.5%, and 216.1% as compared with 2015 levels, respectively, suggesting that the improvements strongly depend on afforestation locations. Driven by the new GGP policy, a high proportion of economic forest increased provisioning service (272.2%), but at the expense of decreases in soil retention (−25.1%), flood mitigation (−11.4%), water purification (−36.6%), and carbon storage (−48.5%). We identified a suitable scenario that would reduce the trade-offs, which associated with afforestation types and their spatial allocation. Identifying priority areas of afforestation types can inform the GGP policy to assure sustainable and broader benefits.