Ca1-x Sr1-xEu2xSiO4 (CaSrSiO4:Eu2+) phosphors were prepared by a novel aqueous solution technique using propylene glycol-modified silane (PGMS), combined with a freeze-drying process. The precursors were heat-treated under a reducing atmosphere with BaCl2 flux. X-ray diffraction indicated that the obtained phosphors exhibited an α0-CaSrSiO4 structure. The wavelength at the phosphors' maximum emission was systematically shifted beyond 600nm as the Eu26 concentration was increased. The corresponding excitation spectra were extended to the visible light region (400-500 nm) with increasing Eu 2+ concentration. These results implied that CaSrSiO 4:Eu2+ is a red-emitting phosphor excited by near-UV and blue-light-emitting diodes.