A series of Eu3+ singly- and Dy3+/Eu3+ co-doped CaLaGa3O7 single matrix phosphors were successfully prepared by high-temperature solid-phase method. The phase and luminescence properties of the samples were characterized by X-ray diffraction (XRD) and photoluminescence spectra. The XRD patterns show that all the prepared samples have a tetragonal structure consistent with the matrix crystal, indicating the successful synthesis of that Eu3+ singly- and Dy3+/Eu3+ co-doped CaLaGa3O7 phosphors. Under excitation of 393 nm, Eu3+∶CaLaGa3O7 exhibits characteristic red emission of Eu3+ (5D0→7F2), and the luminescence purity is as high as 100%. After introducing Dy3+, Dy3+/Eu3+ co-doped CaLaGa3O7 phosphors could be excited not only by 393 nm light but also by 348 nm. Regardless of the excitation wavelength, the emission spectra of Dy3+/Eu3+∶CaLaGa3O7 include both the characteristic red emission of Eu3+ and the yellow emission of Dy3+ (4F9/2→6H13/2). By analyzing the emission spectra and fluorescence lifetime, it is confirmed that there exists effective energy transfer process between Dy3+ and Eu3+ in the co-doped phosphors. Further, the corresponding chromaticity coordinates and CCT values were calculated. The results show that the overall chromaticity coordinates shift from the yellow-green region to the yellow-orange region when the excitation wavelength is changed from 348 nm to 393 nm. Therefore, the Dy3+/Eu3+∶CaLaGa3O7 is a tunable luminescent material with good application prospects in displays and solid-state lighting.