In this work, LaPO:Ce, Tb phosphors were prepared by firing a LaPO:Ce, Tb precipitate using an ionic-liquid-driven supported liquid membrane system. The entire system consisted of three parts: a mixed rare earth ion supply phase, a phosphate supply phase, and an ionic-liquid-driven supporting liquid membrane phase. This method showed the advantages of a high flux, high efficiency, and more controllable reaction process. The release rate of PO from the liquid film under different types of ionic liquid, the ratio of the rare earth ions in the precursor mixture, and the structure, morphology, and photoluminescence properties of LaPO:Ce, Tb were investigated by inductively coupled plasma-atomic emission spectroscopy, X-ray diffraction, Raman spectra, scanning electron microscopy, and photoluminescence emission spectra methods. The results showed that a pure phase of lanthanum orthophosphate with a monoclinic structure can be formed. Due to differences in the anions in the rare earth supply phase, the prepared phosphors showed micro-spherical (when using rare earth sulfate as the raw material) and nanoscale stone-shape (when using rare earth nitrate as the raw material) morphologies. Moreover, the phosphors prepared by this method had good luminescent properties, reaching a maximum emission intensity under 277 nm excitation with a predominant green emission at 543 nm which corresponded to the D-F transition of Tb.