In this study, we report on the alignment properties of nematic liquid crystals on various transparent structured sapphire layers formed by laser-induced periodic surface structures (LIPSS). One-dimensional LIPSS (1D-LFSL) are generated by infrared femtosecond laser pulses along parallel lines covering an area of 5 × 5 mm2, with a line spacing that is varied between 7 and 17 µm. These periodic structures, employed as alignment layers, have a spatial periodicity of about 980 nm, a modulation depth of about 100 nm, and exhibit a high quality due to being characterized by a high degree of homogeneity and parallelism of the structured features. It is found that such alignment layers of the sapphire surface lead to a decreasing azimuthal anchoring energy, when the width of the unstructured gap is increased. Modifying the sapphire surface by an ITO-coating with further deposition of a polyimide film increases the azimuthal anchoring energy by a factor of about four up to Wφ ~ 4.25 × 10−6 J/m2, when the minimum width of the unstructured gap is 7 µm. Comprehensive measurements and comparisons of the azimuthal anchoring energy as well as the pretilt angle for the 1D-LFSL, unstructured gaps, and entire areas depending on the width of unstructured gaps are presented and discussed.