In this paper, we propose a new concept for the material design for near-ultraviolet (UV)-excited narrow-band phosphors with f−f emissions by bandgap engineering. The perovskite oxide−oxynitride solid solutions, namely, CaTa 1−x Zr x O 2+x N 1−x , were used as host materials to demonstrate our design principle. Photoluminescence (PL) excitation and emission control were systematically performed on Pr 3+ -activated CaTa 1−x Zr x O 2+x N 1−x , where x is in the range of 0.0−1.0. Tuning the PL excitation wavelength was archived over a large wavelength range by tailoring the bandgap of CaTa 1−x Zr x O 2+x N 1−x with different Ta/Zr and N/O ratios. Notably, an intense red emission from Pr 3+ was observed at 614 nm under the near-UV irradiation of 375 nm when the bandgap of the host material CaTa 1−x Zr x O 2+x N 1−x (x = 0.75) was approximately 3.0 eV. Such a red emission peak was assigned to the electron transition between the 1 D 2 and 3 H 4 levels of the Pr 3+ ions. In contrast, when the bandgap was above 3.0 eV, the PL emission spectra were systematically varied with the bandgap of the host materials. Some emission peaks from the electron transition between 3 P 0 and 3 H 4 , 3 H 5 , and 3 F 2 levels were observed in the samples with x = 0.90 and x = 0.95. Our results indicate that the PL properties of the phosphors with f−f emission are systematically controlled based on the bandgap engineering for the host materials.