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A photoalignment material of a PGMAcr, poly[3-(acryloyloxy)-2-hydroxypropyl methacrylate] using a photopolymerized the acrylate unit by photo-initiator and a PGMA4Ch, poly[3- (4-chalconyloxy)-2-hydroxypropyl methacrylate] using a photodimerization by chalcone group were synthesized. Also, the liquid crystal (LC) aligning capabilities on the photopolymer layers were studied. A good LC alignment with UV exposure on the PGMAcr surface can be obtained. However, the LC alignment defects were observed on the PGMA4Ch surface. The LC aligning capabilities of the PGMAcr surface by photo-initiator were better than that of the PGMA4Ch surface by chalcone group as photosensitive moiety.