This study compares the performance of light-emitting cement and polymeric mortars. To accomplish this objective, cement, polyester, and epoxy mortars were prepared with and without strontium aluminate (SrAl2O4: Eu2+ Dy3+) based light-emitting phosphor (LEP). The water absorption, compressive strength, ultrasonic pulse velocity, and luminescence intensity tests were performed to compare and assess the characteristics of LEP-based cement and polymeric mortars. The results show that using strontium aluminate phosphor improved the mechanical performance of cement and polymer-based mortars. Notably, polymeric mortars demonstrate significantly lower water absorption compared to their cement counterparts. Furthermore, afterglow performance investigation confirmed that light-emitting polymeric mortars exhibit more persistent luminosity than cement counterparts. Analytical characterizations employing X-ray diffraction (XRD), scanning electron microscopy, energy-dispersive X-ray spectroscopy (EDX), and Fourier-transform infrared spectroscopy elucidated the effective role of light-emitting phosphors within cement and polymeric matrices. Based on the test results, it is deduced that employing strontium aluminate-based light-emitting phosphor in producing light-emitting polymeric composites could be a promising strategy for sustainable and resilient building design.