Carbonyl sulfide (COS) measurements enable quantification of terrestrial photosynthesis, which cannot be directly measured at scales greater than the leaf level. The accuracy of COS-based estimates of gross primary production (GPP) depends on how we relate the COS uptake to that of CO2. This study shows that COS-based GPP estimates will be significantly overestimated if the different environmental responses of COS and CO2 uptake are not taken into account. These findings are relevant for studies that rely on COS to quantify ecosystem to regional scale GPP, and support the use of a COS-based approach to constrain ecosystem flux partitioning. Moreover, the strong stomatal control on COS uptake shown in this study makes COS a suitable tracer f...