This review introduces recent attempts in the photoalignment processes of liquid crystalline polymers focusing on the two aspects. First, the strategies to ensure effective in-plane alignment of the photoresponsive mesogens are summarized. Despite many investigations reported so far, the film systems have not been optimized for efficient photoreaction. Second, new photoalignable systems involving block copolymer frameworks such as surface-grafted polymers and block copolymer thin films are introduced. The photoalignment processes in such mesoscopic systems involve strong cooperative motions among different hierarchical size features. Based on these approaches, a new strategic platform, photoalignment via a command surface at the free surface, is further proposed.