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Global Navigation Satellite Systems-Reflectometry (GNSS-R) has shown unprecedented advantages to sense Soil Moisture Content (SMC) with high spatial and temporal coverage, low cost, and under all-weather conditions. However, implementing an appropriated physical basis to estimate SMC from GNSS-R is still a challenge, while previous solutions were only based on direct comparisons, statistical regressions, or time-series analyses between GNSS-R observables and external SMC products. In this paper, we attempt to retrieve SMC from GNSS-R by estimating the dielectric permittivity from Fresnel reflection coefficients. We employ Cyclone GNSS (CYGNSS) data and effectively account for the effects of bare soil roughness (BSR) and vegetation optical depth by employing ICESat-2 (Ice, Cloud, and land Elevation Satellites 2) and/or SMAP (Soil Moisture Active Passive) products. The tests carried out with ICESat-2 BSR data have shown the high sensitivity in SMC retrieval to high BSR values, due to the high sensitivity of ICESat-2 to land surface microrelief. Our GNSS-R SMC estimates are validated by SMAP SMC products and the results provide an R-square of 0.6, Root Mean Squared Error (RMSE) of 0.05, and a zero p-value, for the 4568 test points evaluated at the eastern region of China during April 2019. The achieved results demonstrate the optimal capability and potential of this new method for converting reflectivity measurements from GNSS-R into Land Surface SMC estimates. [ABSTRACT FROM AUTHOR]