SiO2/REFP@SAOED long-lasting phosphorescent composite with yellow-reddish emitting color was successfully prepared by coating the red-emitting fluorescent pigment (REFP) on the surface of the green-emitting SrAl2O4:Eu2+, Dy3+ (SAOED) long-lasting phosphor (LLP) via sol-gel technology. The FT-IR spectra, thermal stability, photoluminescence (PL) spectra, afterglow decay properties, quantum yield (QY) and CIE phosphorescent chromaticity coordinates of the SiO2/REFP@SAOED were systematically investigated. The results indicated that the it can withstand 380°C operation without do any harm to its luminescence properties; the PL emission spectra consisted of two parts ranging from 450–575 nm and 576–700 nm, and its intensity in the range of 576–700 nm increased gradually with the increase of REFP. The coated REFP had a negative effect on the afterglow brightness of the SAOED, and the brightness value decreased gradually with the increase of REFP as well. The QY of SiO2/REFP@SAOED was a combination of the SAOED and the REFP, and it decreased to 25.1% when the concentration of the REFP was added to 0.9%. The phosphorescent color the SiO2/REFP@SAOED tended to red-shift with the increase of the REFP, and showed a yellow-reddish color when the concentration of the REFP was 0.9%.