We proposed a method for enhancing the planar orientation of reactive mesogen (RM) molecules by means of anisotropic plasma treatment. Anisotropic surface plasma, of which energy density is dependent on the azimuthal angle, was generated by column-shaped ceramic electrodes. The anisotropic plasma was discharged on the surface of a polyvinyl alcohol (PVA) alignment layer before the rubbing process began. The contact angle of the surface was increased from 12° to 83° after plasma treatment, indicating a hydrophobic property of the surface. From the atomic force microscopy (AFM) measurement, it was found that the grain size of the PVA layer was reduced and that the grooved patterns were formed provided that the plasma direction was parallel to the rubbing direction of the surface. Consequently, the planar orientation was enhanced, and the in-plane retardation of the photo-polymerized RM films increased when the parallel plasma was treated on the surface.