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Surface enhanced Raman scattering (SERS) spectroscopy was first utilized to study the photo-orientation behaviour of the photoreactive groups on a novel photo-alignment film surface and elucidate the generation mechanism of pretilt angle. The novel photo-alignment film was prepared by spin-coating a solution of ladderlike polysiloxane (LPS)bearing dual photoreactive group on an ITO surface and by irradiation with linear-polarized ultraviolet (LPUV) light. A Si-H terminal compound (M) containing an identical photosensitive part has been used to fabricate a model film for SERS investigation.