This paper presents a study on the estimation of water content of oilsands tailings using spectral reflectance measurements in the solar range (350–2500 nm). Spectral measurements were collected in the laboratory from two types of tailings namely Mature Fine Tailings (MFT) and samples from a Tailings Solvent Recovery Unit (TSRU). Several spectral features such as absolute reflectance, depth of the absorption features at 1450 and 1925 nm, Normalized Soil Moisture Index (NSMI), and wavelength shift of the 1900 nm absorption band were derived and their correlation with measured gravimetric moisture content was assessed. Results show that for the moisture regime beyond 15% water content, all the examined parameters show a good correlation with water content (R2 > 0.78). Below 15% moisture levels, however, the capability of most of the spectral estimators to measure moisture content dramatically decreases.