This work reports an alternative method for determining thermal degradation of graphite-based thin film hydrophobic coatings using the D and G graphite vibrations as a probe. We show that the Raman spectrum of the coating as a function of temperature is an efficient probe for detecting changes in the surface properties. Both D and G bands of graphite are sensitive to changes of the coating matrix induced by temperature. We apply the Raman technique to correlate the changes of D and G vibrations with those found by different experimental methods such as contact angle measurements and thermogravimetric analysis to characterize organosilane hydrophobic coatings.