Abstract— A plasma‐beam process, developed for the alignment of liquid crystals (LC) in electro‐optic applications, has been successfully applied to align “non‐standard” LC, such as crystalline materials with LC phases at elevated temperatures and reactive mesogenes. In addition to the high alignment quality of the materials, there is no need for an intermediate layer between the substrate and the LC layer. Furthermore, the construction of our source simplifies the alignment procedure of large‐area rigid substrates and the roll‐to‐roll processing of flexible films. This method opens new horizons for optical retarders and polarizers, as well as anisotropic semiconducting films for organic electronics.