Perovskite light‐emitting diodes (Pero‐LEDs) have attracted significant attention due to their high color purity and solution processing, presenting potential applications for next‐generation solid‐state lighting and displays. Continued materials development has shown that passivating non‐radiative defects can improve device performance. In theory, CsPbBr3&Cs4PbBr6 should be a model emitter for Pero‐LEDs, as its lattice matching provides ideal passivation and efficient exciton confinement. However, the low charge transport of Cs4PbBr6 has so far hindered device performance. Herein, a dual‐phase regulation method to grow a CsPbBr3&Cs4PbBr6 perovskite layer that enables efficient electrical injection is developed. This leads to the realization that Pero‐LEDs with a maximum EQE of 22.3% with a luminance of 10,050 cd m−2, and the devices show a T50 of 59 h at 130 cd m−2.