A tremendous potential has been observed in the designing of long afterglow materials for sensing, bioimaging, and encryption applications. In this study, two different strontium aluminate-based luminescent materials; SrAl2O4: Eu, Dy (S1), and Sr4Al14O25: Eu, Dy (S2) were melt-mixed with polypropylene (PP) matrix, and the phosphorescence properties were evaluated. After excitation at 320 nm, the PP/S1 composite exhibited a green emission and the PP/S2 generated a blue emission at 520 nm and 495 nm, respectively. The emission spectra intensity increased by increasing the content of these luminescent fillers. The attenuated total reflection-Fourier transform infrared (ATR-FTIR) experiments show that no chemical reaction occurred during the melt-mixing process. The differential scanning calorimetry (DSC) results revealed that the total crystallinity of the composites reduced by increasing the amount of the fillers; however, no changes in the temperature of melting (Tm) and crystallization (Tc) of PP were observed. Both fillers improved the impact strength of the composites, but the tensile strength (TS) and modulus (TM) decreased. Poly (ethylene glycol) dimethyl ether (P) plasticizer was used to improve the filler-matrix interaction and its dispersion; nevertheless, it adversely affected the intensity of the luminescence emissions.