Tm3+ or Er3+ ions individually doped CaLa2ZnO5 (CLZO) phosphors were synthesized by a citrate sol–gel method. The phase formation and morphological properties of these phosphors were analyzed by X-ray powder diffraction patterns and scanning electron microscope images, respectively. Under ultraviolet (UV) or near UV light excitations, the luminescence properties of these phosphors were studied as a function of Tm3+ or Er3+ ion concentration. Likewise, cathodoluminescence properties were measured as a function of accelerating voltage and filament current. The CLZO:Tm3+ phosphor revealed the intense blue emission due to the 1D2→3F4 electronic transition and the CLZO:Er3+ phosphor exhibited the green emission due to the 4S3/2→4I15/2 electronic transition. The decay curves of these phosphors were well fitted to a single exponential function. The chromaticity coordinates were calculated for the synthesized CLZO:Tm3+ and CLZO:Er3+ phosphors.