Light‐emitting diodes (LEDs) are widely used in lighting and display applications. Carbon quantum dots (CQDs), which have high biocompatibility, high resistance to photobleaching, and full‐spectrum luminescence, have inherent advantages as fluorescent materials for LED devices. Herein, multicolor CQDs are prepared by a new reagent engineering strategy due to the difference of effective conjugate length and the surface electron‐withdrawing groups of CQDs. White CQDs are realized by mixing blue, green, and red CQDs proportionally. Then, the aggregation‐caused quenching phenomenon of CQDs is suppressed through the hydrogen‐bonding network of cellulose nanofibrils (CNFs). Multicolor fluorescent films are prepared from CQDs and CNFs by simple mixing and casting methods. Finally, thin‐film encapsulation based on the photosensitive resin ABPE‐10 coating can be realized and rapidly assembles into fluorescent films with different light‐emitting colors into LED devices, leading to have superior thermal performance compared with conventional LEDs. White LEDs have excellent white‐light illumination performance, with Commission Internationale de L’Eclairage color coordinates of (0.33, 0.37), a correlated color temperature of 5688 K, and a color rendering index of 86. This strategy provides a convenient and scalable pathway for low‐cost, environmentally friendly, and high‐performance CQDs‐based LEDs.
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