Recent studies have shown the promise of remotely sensed solar‐induced chlorophyll fluorescence (SIF) in informing terrestrial carbon exchange, but analyses have been limited to either plot level (~1 km2) or hemispheric/global (~108 km2) scales due to the lack of a direct measure of carbon exchange at intermediate scales. Here we use a network of atmospheric CO2 observations over North America to explore the value of SIF for informing net ecosystem exchange (NEE) at regional scales. We find that SIF explains space‐time NEE patterns at regional (~100 km2) scales better than a variety of other vegetation and climate indicators. We further show that incorporating SIF into an atmospheric inversion leads to a spatial redistribution of NEE estimates over North America, with more uptake attributed to agricultural regions and less to needleleaf forests. Our results highlight the synergy of ground‐based and spaceborne carbon cycle observations.