AbstractDispersible and functionalizable long persistent luminescent (LPL) materials are highly desired for flexible use of LPL in various fields. However, synthesizing metal‐free LPL systems with stable long‐lived intermediates and reactive surface groups, which are key requirements for robust LPL and the ability to be functionalized, has proven to be challenging. Herein, the microwave‐assisted preparation of carbon dots (CDs)‐based LPL materials is demonstrated with abundant surface amino groups via in situ embedding of CDs into carbon nitrides (CNs). The incorporation of CDs leads to the formation of deep traps and promotes exciton transmission between CDs and trap states, contributing to the generation of LPL. By varying the embedded CDs, tunable LPL ranging from blue to yellow can be achieved, with a duration exceeding 10 min. Due to the covalent bonding between CDs and CNs, the materials (named CDs@CNs) exhibit robust LPL under ambient conditions and evenly dispersed in water through ultrasonic treatment. Furthermore, the surface amino groups serve as sites for further modification, allowing for on‐demand performance design and control, such as adjustable hydrophilicity–hydrophobicity for various applications. This work provides new insights into designing superior flexible CDs‐based LPL materials and expanding the domain of metal‐free LPL materials.
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