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Chromium-doped α-alumina is naturally photo-luminescent with spectral properties that are characterized by R-lines with two distinct peaks known as R1 and R2. When the material is subjected to stress, shifts in the R-lines occur, which is known as the piezospectroscopic (PS) effect. Recent work has shown that improved sensitivity of the technique can be achieved through a configuration of nanoparticles within a polymer matrix, which can be applied to a structure as a stress-sensing coating. This study demonstrates the capability of PS coatings in mechanical tests and investigates the effect of nanoparticle volume fraction on sensing performance. Here, measurements of spectral shifts that capture variation in stress of the coating during mechanical testing and in the region of substrate damage showed that stress contours are more noticeable on a soft laminate than hard laminate. It was found that the 20 % volume fraction PS coating showed the most distinct features of all the coatings tested with the highest signal-to-noise ratio and volume fraction of α-alumina. Post failure assessment of the PS coatings verified that the coatings were intact and peak shifts observed during mechanical testing were due to the stress in the substrate. The results suggest the ability to design and tailor the “sensing” capability of these nanoparticles and correlate the measured stress variations with the presence of stress and damage in underlying structures. This study is relevant to nondestructive evaluation in the aerospace industry, where monitoring signs of damage is of significance for testing of new materials, quality control in manufacturing and inspections during maintenance.