The carbon cycle of the terrestrial biosphere plays a vital role in controlling the global carbon balance and, consequently, climate change. Reliably modeled CO2 fluxes between the terrestrial biosphere and the atmosphere are necessary in projections of policy strategies aiming at constraining carbon emissions and of future climate change. In this study, SMOS (Soil Moisture and Ocean Salinity) L3 soil moisture and JRC-TIP FAPAR (Joint Research Centre—Two-stream Inversion Package Fraction of Absorbed Photosynthetically Active Radiation) data with respective original resolutions at 10 sites were used to constrain the process-based terrestrial biosphere model, BETHY (Biosphere, Energy Transfer and Hydrology), using the carbon cycle data assimilation system (CCDAS). We find that simultaneous assimilation of these two datasets jointly at all 10 sites yields a set of model parameters that achieve the best model performance in terms of independent observations of carbon fluxes as well as soil moisture. Assimilation in a single-site mode or using only a single dataset tends to over-adjust related parameters and deteriorates the model performance of a number of processes. The optimized parameter set derived from multi-site assimilation with soil moisture and FAPAR also improves, when applied at global scale simulations, the model-data fit against atmospheric CO2. This study demonstrates the potential of satellite-derived soil moisture and FAPAR when assimilated simultaneously in a model of the terrestrial carbon cycle to constrain terrestrial carbon fluxes. It furthermore shows that assimilation of soil moisture data helps to identity structural problems in the underlying model, i.e., missing management processes at sites covered by crops and grasslands.