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Organic afterglow materials based on carbon dots (CDs) have aroused extensive attention for their potential applications in sensing, photoelectric devices, and anticounterfeiting. Effective methods to control the CD structure and modulate the energy levels are critical but still challenging. Here, we demonstrate a method to modulate the afterglow emission of CDs@SiO2 composites by controlling the carbonization degree of CDs with variable calcining temperatures. The CDs@SiO2-Raw prepared with a hydrothermal bottom-up synthesis method shows a more polymerized structure of CDs with low carbonization degree, which emits long-lived thermally activated delayed fluorescence (TADF) with the lifetime of 252 ms. After calcination at 550 °C, CDs@SiO2-550 exhibits a larger conjugated π-domain structure with higher carbonization degree, thus inducing room-temperature phosphorescence (RTP) emission with a lifetime of 451 ms. The transformation of the carbonization degree of CD structures leads to changes in energy levels and ΔE ST, which affect their afterglow luminescence behaviors. This work proposes a new concept to modulate the afterglow emission of CDs@SiO2 composites and forecasts potential applications of CD-based afterglow materials.

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