Mechanoluminescence (ML) materials as a special type of energy conversion medium play an important role in a wide range of fundamental applications. However, in numerous previously investigated ML host systems, effective activation of ML was typically confined to limited types of luminescent centers, seriously restricting the emission spectral diversity form a single system. Additionally, a significant proportion of the ML materials identified to date necessitate pre-irradiation with light to acquire ML capabilities. These limitations considerably restrict the practical application of ML in real-world scenarios. Herein, a mechanical-energy-driven piezoelectric gallate system (Ca₃Ga₄O₉) was identified as a promising ML matrix due to its non-pre-irradiation activation properties and excellent lanthanide ion holding capacity. Under non-pre-irradiation conditions, tunable and extended ML spectral domain from violet to near …