A photo-dielectric effect (i.e., a change in dielectric permittivity due to photo-irradiation) has been demonstrated in LaAl0.99Zn0.01O3-delta. Photo-irradiation with an incident energy of 3.4 eV was found to enhance the dielectric permittivity in LaAl0.99Zn0.01O3-delta over a wide frequency range from 100 Hz to 1MHz. The change in dielectric permittivity in the high-frequency region hardly depended on frequency and was not accompanied by an increase in dielectric loss, indicating an intrinsic photodielectric effect in LaAl0.99Zn0.01O3-delta that is not due to photo-conduction. The dependence of the photo-dielectric effect on incident energy suggests the existence of deep in-gap states introduced by Zn substitution. The mechanism of the photo-dielectric effect in LaAl0.99Zn0.01O3-delta relates to the dielectric response of the photo-excited electrons trapped in the deep in-gap states, which work as effective polar displacements under an applied electric field. These findings are expected to contribute to the development of photo-capacitors that enable the remote control of the dielectric response via photo-irradiation. Published by AIP Publishing.