Friction-deposited layers of atactic polystyrene (PS) on inert and OHgrafted gold substrates were the subject of this study to establish a relationship between the friction process and the resulting anisotropy of the transferred polymer chains. We show, by using polarization-modulation infrared reflection-absorption spectroscopy that the deposited PS chains involve an anisotropy in which PS main backbone is rather perpendicular to the friction support, fact that is surprising when compared with the majority of polymers where the anisotropy is along the sliding direction. Moreover, our calculation of the orientation angles revealed that PS chains are more perpendicular in the transferred layers than in spin-coated films. This particular anisotropy is probably due to a parallel reorientation of the phenyl ring on the friction support whatever the surface chemistry is. On the other hand, this study was useful to rectify the assignment of infrared bands unclearly reported in the literature. (c) 2006 Wiley Periodicals, Inc.