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This study not only opens new avenues for biodetection, but also provides deep insights into how molecules modulate laser light at the biointerface, laying the foundation for the development of smart bio-photonic devices at the molecular level.Micellar and vesicular structures capable of sensing and reporting the chemical environment as well as facilely introducing user-defined functions make a vital contribution to constructing versatile compartmentalized systems. Herein, by combining poly(ionic liquid)-based photonic spheres and an etc