the piezoelectric effect and induced by mechanical vibration. [1][2][3][4] Recently, it has been rapidly attracting the attention of researchers, because of its promising potential toward sustainable energy-saving technologies including self-driven electronics and power-less displays. [5,6] Generally, a composite structure has been adopted in which ML-active materials such as zinc sulfide (ZnS) microparticle (MP) phosphors are embedded into elastic polymer matrices such as polydimethylsiloxane (PDMS), denoted as a classical ML matrix (CMM), to effectively utilize the novel light-emitting properties with sufficient reproducibility and durability. [7][8][9] Because of its simplicity in processing, the CMM has, indeed, readily enabled a wide range of next-generation applications directed with ubiquitous electronics such as pressure-sensitive light-emitting devices, [10][11][12] skin-motion sensors, [13] selflighting fabrics and displays. [14][15][16] For lighting and imaging applications, demonstration of primary colors-red (R), green (G), and blue (B)-with high spectral accuracy (peak wavelength position) and purity (full-width at half-maximum (FWHM)) is a key point as their appropriate combinations for full-color implementation, including white (W) light. Significant advances and scientific backgrounds regarding the realization of full-color light have been established in the electroluminescent device platform, attributed to the development of pure R/G/B color emitters. [17,18] Targeted to a high-quality full-color implementation in the ML system, by employing the key principles learned from the electroluminescent systems, recent endeavors have demonstrated a color gamut from pale G to orange in the CMM platform using spectrally color-pure ML-active materials. [12,16] Nevertheless, the full-color implementation of ML, even in the recent ML technology, still lags far behind. This is attributed to the intrinsic limitation of the MLactive materials, in which the emission characteristics (particularly, the peak wavelengths and the FWHMs in ML spectra) and colors are largely determined by the metal ion dopants. In addition, the doping process of the materials usually requires elevated temperature and/or reactive atmosphere, further disrupting the research toward full-color demonstration more challenging. [19][20][21] To challenge the inherent drawbacks of the CMM-based platform and toward the realization of pure-and full-color