Tb(3+), Tm(3+), and Dy(3+)-activated SrY2O4 phosphors have been prepared via Pechini-type sol-gel method. X-Ray diffraction (XRD), field-emission scanning electron microscopy (FE-SEM), transmission electron microscopy (TEM), photoluminescence (PL) and lifetimes, as well as cathodoluminescence (CL) spectra were used to characterize the samples. Under low-voltage electron beam excitation, the Tb(3+)-doped samples show a green luminescence, with a better CIE coordinates and higher emission intensity than the commercial product ZnO: Zn. Blue and yellow emissions could be obtained by doping with Tm(3+) and Dy(3+), respectively. A color-tunable emission in SrY2O4 phosphors can be realized by co-doping with Tm(3+) and Dy(3+). White cathodoluminescence (CL) has been realized in a single-phase SrY2O4 host by co-doping with Tm(3+) and Dy(3+) for the first time with CIE (0.315, 0.333). Furthermore, the cathodoluminescence (CL) properties of SrY2O4: Tb(3+)/Tm(3+)/Dy(3+) phosphors including the dependence of CL intensity on accelerating voltage and filament current, the decay behaviour of CL intensity under electron bombardment, and the stability of CIE chromaticity coordinate have been investigated in detail. The as-prepared phosphors might be promising for use in field-emission display (FED) devices.