Gadolinium aluminate is an effective host for doping with various ions, and it can emit various colors. However, it is not easy to prepare transparent ceramics of gadolinium aluminate using traditional methods, although transparent ceramics are very suitable for solid lighting. In this work, a two-dimensional guidance strategy has been successfully carried out for perovskite-structured aluminate ceramic film. Through the two-dimensional interfacial reaction, GdAlO3:Eu3+ (GAP:Eu3+) transparent ceramic films were successfully fabricated using nanosheets exfoliated from layered gadolinium hydroxide, a rare earth source. The final films were tested by characterization techniques, including XRD, SEM, TEM, FT-IR, PLE/PL spectroscopy, temperature-dependent PL spectroscopy, and luminescence decay analysis. The perovskite film of transparent ceramics can be obtained by calcining LRH nanosheets on the substrate of amorphous alumina at 1550 °C in air with a reaction time of 2 h. During the interface reaction, temperature-dependent element diffusion takes the dominant role, and increased reactants take in the reaction with increasing calcination temperature. The grain for ceramic film is only 2–5 μm, which is much smaller than that for bulk ceramic. This is mainly due to the lower temperature and the interface diffusion. Ceramic film has a high transmittance larger than 90% at the visible range. Upon UV excitation at 254 nm, the film exhibits intense emission at the red wavelength range. The outcomes described in this work may have wide implications for transparent ceramics and layered rare-earth hydroxides.