Diamond-like carbon (DLC) films without H deposited with a DC magnetron in-line sputtering system have shown sufficient self-alignment properties towards liquid crystals (LC). The DLC film was successfully used as an alignment layer for LC without any alignment processes such as rubbing or atomic beam bombardment or UV irradiation. From the observations of the test cells, the LC director was aligning parallel to the substrate movement direction of the in-line sputtering system. The alignment property of the DLC films has been demonstrated by a contrast ratio value of close to 200. It appears that DLC film may have anisotropic structure that is interacting with LC to align.