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Abstract Stimuli‐responsive materials that exhibit circularly polarized luminescence (CPL) have attracted significant attention for applications in chiroptical sensing and information security. However, the development of CPL platforms remains limited owing to the challenges in chirality control, reliance on photoexcitation, and complexity of the decoding mechanisms. In this paper, a force‐insensitive chiroptical platform is presented, constructed by integrating a mechanoluminescent phosphor layer with a photonic crystal layer. The phosphor layer enables both photoluminescence (PL) and mechanoluminescence (ML) emissions, whereas the photonic crystal layer enables tunable photonic bandgaps, achieved by adjusting the cellulose nanocrystal‐to‐glucose ratio. This structural design enables modulated CPL with high dissymmetry factors ( g lum ), reaching −0.512 and −0.573 for g PL and g ML , respectively. Further, the system shows distinct solvent‐responsive circularly polarized mechanoluminescence (CPML) behavior. Moreover, its force‐insensitive response offers a robust and light‐free strategy for information decryption, significantly enhancing security while simplifying operation. These findings highlight the potential of the CPML platform for next‐generation chiroptical sensing and secure information technologies.
Nie et al. (Fri,) studied this question.