Controlling the alignment of various functional molecules is important for the development of many next-generation, high-performance optical devices. However, there are some limitations in inducing molecular alignment using the current methods. We report herein the alignment control of azobenzene in a polymer film by a simple, new alignment-patterning technique based on a scanning wave photopolymerization (SWaP) concept. In this technique, molecular alignment was induced by the spatiotemporal control of the non-polarized light. A photoisomerizable azobenzene molecule, Disperse Red 1 (DR1), was doped into the photopolymerizable mixture, and it was successfully aligned along the direction of the neighboring mesogens; the alignment was induced by SWaP with unpolarized light. The alignment behavior showed that the degree of photoisomerization of the doped azobenzene moieties was proportional to the light intensity, and the unidirectional alignment of DR1 was achieved through optimization of the photopolymerization conditions. This finding indicates that SWaP could be employed as a novel and simple fabrication process for preparing a wide variety of highly functional optical devices requiring alignment control. The alignment of azobenzene molecule was induced by a new-alignment-patterning technique based on a scanning wave photopolymerization (SWaP) concept with unpolarized light. This finding indicates that SWaP could be employed as a novel and simple fabrication process for preparing a wide variety of highly functional optical devices requiring alignment control.