We have investigated the photoregulation occurring in monolayer systems mixed with monolayers of poly(vinyl alcohol)s bearing azobenzene sides (6Az5PVA) and liquid crystal (LC). For a mixed monolayer system with trans-6Az5PVA and LC mesogenic molecules, transient-displacement-current pulses originating in the orientational change of the LC mesogenic molecules were not observed, although transient-displacement-current pulses due to the photoisomerization of 6Az5PVA monolayers were detected for a monolayer system mixed with LC mesogenic molecules possessing dielectric anisotropy. In contrast, for a cis-6Az5PVA monolayer mixed with LC mesogenic molecules, transient-displacement-current pulses originating in the orientational change of LC mesogenic molecules were observed during the initial photoirradiation cycle with visible light.