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Carbon nanodots (CDs) have emerged as an alternative option for traditional nanocrystals due to their excellent optical properties and low toxicity. Nevertheless, high emission efficiency is a long‐lasting pursuit for CDs. Herein, CDs with near‐unity emission efficiency are prepared via atomic condensation of doped pyrrolic nitrogen, which can highly localize the excited states thus lead to the formation of bound excitons and the symmetry break of the π–electron conjugation. The short radiative lifetimes (<8 ns) and diffusion lengths (<50 nm) of the CDs imply that excitons can be efficiently localized by radiative recombination centers for a defect‐insensitive emission of CDs. By incorporating the CDs into polystyrene, flexible light‐converting films with a high solid‐state quantum efficiency of 84% and good resistance to water, heating, and UV light are obtained. With the CD–polymer films as light conversion layers, CD‐based white light‐emitting diodes (WLEDs) with a luminous efficiency of 140 lm W−1 and a flat‐panel illumination system with lighting sizes of more than 100 cm2 are achieved, matching state‐of‐the‐art nanocrystal‐based LEDs. These results pave the way toward carbon‐based luminescent materials for solid‐state lighting technology. [ABSTRACT FROM AUTHOR]