The photoalignment of liquid crystalline azobenzene-containing polymers has been an active area of research, which intends to apply for optical elements such as rewritable optical memory, photorefractive and photomechanical devices. However, the photoalignment behavior is hardly studied in nano-confined environments. We introduce herein our current activities on the new types of photoalignment controls of azobenzene-containing liquid crystalline polymer materials; (i) polymer chains tethered (grafted) onto a substrate and (ii) nanostructures formed by a block copolymer. New platforms for the photoalignment technologies are anticipated in these photoactive thin film systems.