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Background and aims: The quantitative retrieval of soil organic carbon (SOC) storage, particularly for soils with a large potential for carbon sequestration, is of global interest due to its link with the carbon cycle and the mitigation of climate change. However, complex ecosystems with good soil qualities for SOC storage are poorly studied. Methods: The interrelation between SOC and various vegetation remote sensing drivers is understood to demonstrate the link between the carbon stored in the vegetation layer and SOC of the top soil layers. Based on the mapping of SOC in two horizons (0–30 cm and 30–60 cm) we predict SOC with high accuracy in the complex and mountainous heterogeneous páramo system in Ecuador. A large SOC database (in weight % and in Mg/ha) of 493 and 494 SOC sampling data points from 0–30 cm and 30–60 cm soil profiles, respectively, were used to calibrate GPR models using Sentinel-2 and GIS predictors (i.e., Temperature, Elevation, Soil Taxonomy, Geological Unit, Slope Length and Steepness (LS Factor), Orientation and Precipitation). Results: In the 0–30 cm soil profile, the models achieved a R2 of 0.85 (SOC%) and a R2 of 0.79 (SOC Mg/ha). In the 30–60 cm soil profile, models achieved a R2 of 0.86 (SOC%), and a R2 of 0.79 (SOC Mg/ha). Conclusions: The used Sentinel-2 variables (FVC, CWC, LCC/Cab, band 5 (705 nm) and SeLI index) were able to improve the estimation accuracy between 3–21% compared to previous results of the same study area. CWC emerged as the most relevant biophysical variable for SOC prediction. [ABSTRACT FROM AUTHOR]