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Compared with green and red perovskite light‐emitting diodes (PeLEDs), the development of blue PeLEDs has been lagging due to high defect density and inferior carrier transport. Herein, a novel defect‐passivation strategy is proposed to fabricate efficient sky‐blue PeLEDs by using isocyanate molecules. This strategy not only significantly reduces the nonradiative recombination loss caused by defects...