Surface-enhanced Raman scattering (SERS) and tip-enhanced Raman scattering (TERS) are fast, convenient, and non-destructive molecular detection techniques, which provide a practical method for studying interfacial reactions with high resolution and accuracy. Both techniques are able to provide quantitative and qualitative information on the chemical properties, conformational changes, order state, and molecular orientation of various surfaces. This paper aims at summarizing the research efforts in the field of SERS and TERS related to tribological systems with a special emphasis on thin film and nanoparticles. This overview starts with a brief introduction for both techniques. Afterwards, it summarizes pros and cons of both techniques related to the advanced characterization of tribologically induced reactions layers. Moreover, the feasibility of both techniques to evaluate the friction and wear performance of new lubricant additives including solid lubricants is discussed. At the end of this review article, the main challenges and future directions in this field are prospected to emphasize the development direction of SERS and TERS in tribology and lubricants. Lubricants 2019, 7, 81 2 of 16For this purpose and depending on the material used, various techniques including white light interferometry and laser scanning microscopy (surface topography), Raman spectroscopy, Sum frequency generation (SFG) spectroscopy, X-ray photoelectron spectroscopy and infrared-spectroscopy (surface chemistry) as well as X-ray diffraction, electron backscatter diffraction and transmission electron microscopy (microstructure) can be utilized. It needs to be emphasized that a multi-method approach is recommendable since only one characterization technique will never be able to reveal the full picture regarding the desired information [12].Apart from the fact that there is no powerful in-situ characterization technique to assess any of this information during sliding/rubbing, the entire situation is further complicated since friction and wear are influenced by effects on different scales ranging from macro-to nanoscale [13,14]. Regarding the macro-scale, fabrication tolerances and design aspects can be named as potential effects influencing the resulting coefficient of friction and wear. Related to the micron-scale, the surface topography and surface roughness mainly affect the resulting nominal and real contact area [15]. In this regard, it must be emphasized that the real contact happens at the asperity level, which is typically sub-micron and on the nanoscale. The contact at the asperity level typically induces rather high contact pressure. This can lead to pressure-induced reactions thus generating sub-surface reaction layers, which may substantially influence the corresponding tribological properties [16]. These aspects unambiguously underline that the effects occurring at the nanoscale also significantly alter the resulting friction and wear performance. Consequently, the aforementioned surface topography, surface chemistry, and m...