In order to develop photochromic materials with persistent afterglow emission, such as concrete and smart windows, electrospun polypropylene nanofibers (PPNF) were incorporated into polyethylene terephthalate (PET) for reinforcement. Nanoparticles of lanthanide-activated strontium aluminum oxide (NLSA) were physically embedded into polyethylene terephthalate films to produce transparent PPNF@PET smart membranes. Electrospinning was utilized to create PPNF, which were subsequently included as a roughening agent into PET membranes. The green coloration detected upon exposing the PPNF@PET film to ultraviolet light was verified by CIE Lab coordinates and photoluminescence analysis. The PPNF@PET hybrids with low quantities of NLSA were found to immediately reverse this emission activity after removing the ultraviolet source, which suggest fluorescence emission. Afterglow photoluminescence was detected at higher phosphor concentrations in PPNF@PET by slow reversibility of the light emission, which suggests glow in the dark emission. After 365 nm of excitation, a 517 nm emission band could be monitored from the PPNF@PET hybrids. The chemical structure and morphology of LSA nanoparticles and PPNF were studied, showing diameters of 80–120 nm and 75–180 nm, respectively. Different analysis methods were employed to examine the morphologies of PPNF@PET membranes. As compared to a NLSA-free polyethylene terephthalate control sample, the PPNF@PET smart membranes demonstrated improved scratch resistance. The hydrophobicity and UV resistance of the PPNF@PET smart membranes were improved with an increase in the concentration of NLSA.