Mechanoluminescence ͑ML͒ in a CaAl 2 Si 2 O 8 :Eu 2+ phosphor was greatly enhanced by partial Sr 2+ substitution for Ca 2+ ; ML intensity reached a maximum at Sr 2+ content of 40 mol %. Moreover, ML was not observed at Sr 2+ content of 80 mol % or higher. To investigate the relationship between ML and the crystal structure, Rietveld refinement of the crystal structures was performed, the results of which suggest that the observed ML enhancement and quenching phenomenon were associated with changes in the crystal lattice and crystal symmetry. Furthermore, the effects of partial Sr 2+ substitution on the structure and photoluminescence characteristics were also investigated, and the emission peak was blueshifted from 428 to 403 nm due to the decrease in the crystal field intensity around Eu 2+ . Based on electroluminescence measurements and the structural properties of the material, a possible mechanism for the enhancement in ML intensity is proposed.Mechanoluminescence ͑ML͒ is an intriguing luminescence phenomenon in which light emission is induced by various mechanical stimuli such as compression, friction, impact, and fracture. 1 The ML phenomenon has been known since the 16th century when it was discovered that crystalline sugar and certain minerals emit light when crushed. A considerable amount of research has focused on the fundamental features of the ML phenomenon. However, practical applications were not investigated until a decade ago, as ML was considered to be a fracture phenomenon and thus only a one-off event.The recently developed ML material SrAl 2 O 4 :Eu 2+ , which exhibits a strong green emission that can be repeatedly induced by weak elastic deformation, was developed by Xu and co-workers a decade ago. 2 This type of ML material has attracted considerable attention due to its potential applications as a stress sensor 3 and excitation source, 4 and many researchers have investigated these new ML materials.To date, several materials exhibiting ML in the elastic deformation region have been successfully developed, including SrAl 2 O 4 :Eu 2+ ͑green͒, 2 ZnS:Mn 2+ ͑yellow͒, 5 and BaTiO 3 -CaTiO 3 :Pr 3+ ͑red͒. 6 Although these phosphors exhibit a strong ML intensity, their luminescence spectra are limited to long wavelengths from green to red. For use as an excitation source, ML materials with a short-wavelength emission are highly desirable for many practical applications. Furthermore, these ML materials still have several problems, for example, the poor water resistance of SrAl 2 O 4 :Eu 2+ and the poor stability of ZnS:Mn 2+ and BaTiO 3 -CaTiO 3 :Pr 3+ . Therefore, it is essential to develop novel ML materials with a short-wavelength emission and superior stability. CaAl 2 Si 2 O 8 :Eu 2+ , which was successfully developed in our most recent studies, 7,8 satisfies both requirements because the material has a short-wavelength emission peak of 428 nm and exhibits superior stability to water. However, the ML intensity of CaAl 2 Si 2 O 8 :Eu 2+ is insufficient for practical use. The purpose of the pr...