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Thermochromic phosphors are intriguing materials for realizing thermochromic behaviors of light-emitting diodes. Here a highly luminescent and stable thermochromic phosphor based on one-dimensional Cu 4 I 6 (4-dimethylamino-1-ethylpyridinium) 2 is reported. This unique ionic copper-iodine chain-based hybrid exhibits near-unity photoluminescence efficiency owing to the through-space charge-transfer character of relevant electronic transitions. More importantly, an alternative mechanism of thermochromic phosphorescence was unraveled, supported by a first principles simulation of concerted copper atom migration in the copper-iodine chain. Furthermore, we successfully fabricate a bright thermochromic light-emitting diode using this Cu 4 I 6 (4-dimethylamino-1-ethylpyridinium) 2 thermochromic phosphor. Our reported flexible ionic copper-iodine chain-based thermochromic luminescent material represents a new type of cost-effective functional phosphor., (© 2022 Wiley-VCH GmbH.)