A novel method of forming an alignment layer of a liquid crystal display device includes the steps of providing a substrate (e.g., a processed silicon wafer, etc.) having an alignment layer material deposited thereon and applying a series of pulses from a pulse laser to anneal portions of the alignment layer material and alter its surface morphology. The method can include the step of depositing the alignment layer material (e.g., a spin-on dielectric including SiO2) over the substrate using a spin-on process prior to laser annealing. Applying the series of laser pulses creates a repetitive pattern of features that facilitate alignment of liquid crystals according to a laser scan trace. Liquid crystal display devices with laser-annealed alignment layer(s) are also disclosed. The alignment layers of the invention are quickly and inexpensively applied and are very robust under prolonged, high-intensity light stress.