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Abstract Solar‐induced chlorophyll fluorescence (SIF) shows enormous promise as a proxy for photosynthesis and as a tool for modeling variability in gross primary productivity and net biosphere exchange (NBE). In this study, we explore the skill of SIF and other vegetation indicators in predicting variability in global atmospheric CO₂observations, and thus global variability in NBE. We do so using a 4‐year record of CO₂observations from NASA's Orbiting Carbon Observatory 2 satellite and using a geostatistical inverse model. We find that existing SIF products closely correlate with space‐time variability in atmospheric CO₂observations, particularly in the extratropics. In the extratropics, all SIF products exhibit greater skill in explaining variability in atmospheric CO₂observations compared to an ensemble of process‐based CO₂flux models and other vegetation indicators. With that said, other vegetation indicators, when multiplied by photosynthetically active radiation, yield similar results as SIF and may therefore be an effective structural SIF proxy at regional to global spatial scales. Furthermore, we find that using SIF as a predictor variable in the geostatistical inverse model shifts the seasonal cycle of estimated NBE and yields an earlier end to the growing season relative to other vegetation indicators. These results highlight how SIF can help constrain global‐scale variability in NBE.