Seasonal dynamics of atmospheric carbonyl sulfide (OCS) at regional and continental scales and plant OCS exchange at the leaf level have shown a close relationship with those for CO2. CO2 has both sinks and sources within terrestrial ecosystems, but the primary terrestrial exchange for OCS is thought to be leaf uptake, suggesting potential for OCS uptake as a proxy for gross primary production (GPP). We explored the utility of OCS uptake as a GPP proxy in micrometeorological studies of biosphere-atmosphere CO2 exchange by applying theoretical concepts from earlier OCS studies to estimate GPP. We partitioned measured net ecosystem exchange (NEE) using the ratio of measured vertical mole fraction gradients of OCS and CO2. At the Harvard Forest AmeriFlux site, measured CO2 and OCS vertical gradients were correlated and were related to NEE and GPP, respectively. Estimates of GPP from OCS-based NEE partitioning were similar to those from established environmental regression techniques, providing evidence that OCS uptake can potentially serve as a GPP proxy. Measured vertical CO2 mole fraction gradients at five other AmeriFlux sites were used to project anticipated vertical OCS mole fraction gradients to provide indication of potential OCS signal magnitudes at sites where no OCS measurements were made. Projected OCS gradients at sites with short canopies were greater than those in forests, including measured OCS gradients at Harvard Forest, indicating greater potential for OCS uptake as a GPP proxy at these sites. This exploratory study suggests that continued investigation of linkages between OCS and GPP is warranted.