Rehabilitation is the key factor for improving soil quality and soil carbon stock after mining operations. Monitoring is necessary to evaluate the progress of rehabilitation and its success, but the use of repeated field surveys is costly and time-consuming at a large scale. This study aimed to monitor the environmental/soil rehabilitation process of an Amazonian sandstone mine by applying spectral indices for predicting soil organic carbon (SOC) stock and comparing them to soil quality index. The studied area has different chronological rehabilitation stages: initial, intermediate, and advanced with 2, 10, and 12 years of onset rehabilitation activities, respectively. Non-rehabilitated (NR) and two native forest areas (RA) were used as controls. Soil samples were analyzed for physical, chemical, and biological attributes. After determination of Normalized Difference Vegetation Index and Bare Soil Index, simple regression analysis comparing these indices with SOC stock showed a good fit (R2 = 0.82). Rehabilitated areas presented higher soil quality index (~1.50-fold) and SOC stock (~10.6-fold) than NR; however, they did not differ of RA. The use of spectral indices was effective for monitoring the soil quality in this study, with a positive correlation between the predicted SOC stock and the calculated soil quality index.