The liquid crystal (LC) geometrical phase optics, which is realized by the high-resolution control of the optical axis orientation in transparent micrometer-thin polymer films, is emerging as a next generation of planar optics. It features pronounced optical properties and stimuli-responsive behaviors, which could introduce appealing and new possibilities for photonic purposes. The development of fabrication techniques producing elements with large aperture sizes and arbitrarily varying molecular orientation is of significance in terms of practical utility. Here, we propose the pulsed polarization patterning technique to create large-aperture and defect-free LC geometrical phase elements. We investigated the capability of the azo photo-alignment material responding to nanosecond laser pulses and the corresponding anchoring behaviors to LCs. The threshold was reduced to one fourth of that under the continuous wave recording. The patterning resolution was found to be enhanced to around 0.71 µm, due to the ultra-fast interaction nature of the photo-alignment material with the polarized light field. We proposed the flying exposure mode to deliver high frequency modulated polarized laser pulses (8 kHz), with the precision stage moving in a uniform velocity for light-field stitching and the servo auto-focusing in the sample normal, enabling the stable and reliable polarization patterning for large aperture sizes. We further report on representative fabrication of LC polarization gratings with an aperture of 4 inch and 99.2% average diffraction efficiency.