Land use change is a main factor of affecting water-related ecosystem services (WESs), critical for managing aquatic ecosystem. Nevertheless, how to establish the connection between realistic land management and optimizing WESs is unclear. To address this issue, we selected a typical ecologically vulnerable area, the Ussuri River Basin in China, as an analyzed domain to reveal the driving mechanism of WESs. Furthermore, four land scenarios were established to unfold the connection between land use and WESs. The results are as follows: from 2000 to 2018, cropland expansion led to increases of nitrogen export (+11.55%) and phosphorous export (+12.50%), along with increased food production (+127.27%) and water yield services (+1.41%). We found that the trade-offs occurred mainly within provisioning services (between water yield and food production) or regulating services (between water purification and soil retention). Regarding future scenarios, the traditional ”Grain for Green” scenario failed to benefit ecosystems, not only increasing the trade-off intensity of ecosystem services, but leading to competitive relationships in WESs. As a result, afforestation may not be an optimal solution for the restoration of degraded ecosystems, especially in water-limited areas. The forestland buffer zone scenario was regarded as the optimal land practice, in which WESs were enhanced significantly and trade-offs were reduced between provisioning services, indicating that tree-planting near waters maintained both ecological benefits and fundamental grain outputs. These results highlighted importance of land management on WESs, offering a prospective evaluation of ecosystem service benefits under future development pathway.