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The future of aerospace structures is highly dependent on the advancement of reliable and high-performance materials, such as composite materials and metals. Innovation in high resolution non-invasive evaluation of these materials is needed for their qualification and monitoring for structural integrity. Aluminum oxide (or α-alumina) nanoparticles present photoluminescent properties that allow stress and damage sensing via photoluminescence piezospectroscopy. This work describes how these nanoparticles are added into a polymer matrix to create functional coatings that monitor the damage of the underlying composite or metallic substrates. Different volume fractions of α-alumina nanoparticles in the piezospectroscopic coatings were studied for determining the sensitivity of the coatings and successful damage detection was demonstrated for an open-hole tension composite substrate as well as 2024 aluminum tensile substrates with a subsurface notch.