Whether and how to synchronously regulate stream water nitrogen (N) and phosphorus (P) concentrations and ratios is a major challenge for sustainable aquatic functions. Soil carbon (C):N:P ratios influence soil N and P stocks and biogeochemical processes that elicit subsequent substantial impacts on stream water N and P concentrations and ratios. Therefore, bridging soil and stream water with ecological stoichiometry is one of the most promising technologies for improving stream water quality. Here, we quantified the ecological stoichiometry of soil and stream water relationships across nine catchments. Soil C:P ratio was the main driver of water quality, showing negative correlations with stream water N and P concentrations, and positive correlations with the N:P ratio in P-limited catchments. We revealed that soil C:P ratios higher than 97.8 mol mol−1 are required to achieve the simultaneous regulation of stream water N and P concentrations below the eutrophication threshold and make algal growth P-limited. Furthermore, we found that the relationships between catchment landscape and soil ecological stoichiometry likely provided practical options for regulating soil ecological stoichiometry. Our work highlights that soil ecological stoichiometry can effectively indicate the amount and proportion of soil N and P losses, and can be intervened through rational landscape planning to achieve sustainable aquatic ecosystems in catchments.