We report the preparation of perfect uniaxially-oriented (Ca0.65Sr0.35)0.997Pr0.002TiO3 phosphor thin films on glass substrates with an oriented Dion–Jacobson perovskite RbLaNb2O7 seed layer prepared using an excimer-laser-assisted metal organic deposition process. The obtained phosphor thin films on the seed layer exhibited perfect uniaxial (010)-orientation below 40 mJ/cm2. At 40 mJ/cm2, the film showed intense red luminescence at 612 nm. The luminance was evaluated to be 14.5 cd/m2 under 300 nm excitation light at 3.5 mW/cm2, and this value was 26% higher than that of unoriented film. Above 45 mJ/cm2, the phosphor thin films had a mud-crack pattern. Thus, the crystal orientation quality and luminescence intensity was lowered. The precise control of preparation conditions is necessary for preparation of heterostructures with good orientation quality.