A magneto-optically active thin film of RbjCok[Fe(CN)6]l⋅nH2O has been prepared using a sequential assembly method. Upon irradiation with light and at 5 K, the net magnetization of the film increased when the surface of the film was oriented parallel to the external magnetic field of 0.1 T. However, when the surface of the film was perpendicular to the field, the net magnetization decreased upon irradiation. The presence of dipolar fields and the low-dimensional nature of the system are used to describe the orientation dependence of the photoinduced magnetization. The ability to increase or decrease the photoinduced magnetization by changing the orientation of the system with respect to the field is a phenomenon that may be useful in future device applications.