The graphitization process of a tetrahedral amorphous carbon (ta-C) film under lubrication was investigated using a laboratory-built in situ Raman tribometer. The coating was lubricated with poly-alpha-olefin (PAO), PAO with an added friction modifier (FM), glycerol mono-oleate (GMO). Friction tests were carried out using a ball-on-disk setup, in which a 19-mm diameter ta-C-coated ball was loaded and rubbed against a steel disk that was immersed in a lubricant solution. In situ optical microscopy and Raman spectroscopy were used to monitor the graphitization process and wear tracks of the ta-C-coated ball. Raman analysis was conducted on the rubbed surface of the rotating ta-C-coated ball when it was located under an objective lens every three minutes during sliding. In this study, the degree of graphitization of the ta-C surface was estimated by calculating the intensity ratio of the D-peak and G-peak (ID/IG) in the Raman spectra of the ta-C film during friction tests with different lubricants. All our results suggest that the friction modifier inhibits the progression of graphitization of DLC films by reducing friction, in other words, reducing the contact temperature, and the wear progression of DLC films under boundary lubrication can be induced by graphitization of DLC surfaces at the sliding contact.