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Long‐persistent phosphorescent smart paints have the ability to continue glowing in the dark for a prolonged time period to function as energy‐saving products. Herein, new epoxy/silica nanocomposite paints were prepared with different concentrations of lanthanide‐doped aluminate nanoparticles (LAN; SrAl2O4:Eu2+,Dy3+). The LAN pigment was firstly coated with silicon dioxide (SiO2) utilizing the heterogeneous precipitation technique to provide LAN‐encapsulated between SiO2 nanoparticles (LAN@SiO2). The epoxy/silica/lanthanide‐doped aluminate nanoparticles (ESLAN) nanocomposite paints were coated on steel. The prepared ESLAN paints were studied by transmission electron microscopy (TEM), Fourier‐transform infrared (FTIR) spectroscopy, scanning electron microscopy (SEM), X‐ray fluorescence (XRF) analysis, and energy‐dispersive X‐ray spectroscopy (EDS). The transparency and coloration properties of the nanocomposite coated films were explored by CIE Lab parameters and photoluminescence spectra. The ultraviolet‐induced luminescence properties of the transparent coated films demonstrated greenish phosphorescence at 518 nm upon excitation at 368 nm. Both hardness and hydrophobic activities were investigated. The anticorrosion activity of the nanocomposite films coated onto mild steel substrates immersed in aqueous sodium chloride (NaCl(aq)) (3.5%) was studied by electrochemical impedance spectroscopy (EIS). The silica‐containing coatings were monitored to exhibit anticorrosion properties. Additionally, the nanocomposite films with LAN@SiO2 (25%) exhibited the optimized long‐lasting luminescence properties in the dark for 90 min. The nanocomposite films showed highly reversible and durable long‐lived phosphorescence.

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