All‐inorganic perovskite nanocrystals (NCs) have been widely used in many fields due to their excellent photoelectric properties. However, the instability of their structure and the high lead content need to be solved. Herein, the concept of “High‐entropy” is introduced into NCs to prepare High‐entropy perovskite Cs(Pb1/3Mn1/3Ni1/3)Br3 NCs by high‐energy ball milling method. The effects of milling time and doping ratio of B‐site elements on the structure and performance of perovskite NCs are studied. It is found that Mn2+ and Ni2+ successfully enter the lattice of Pb2+ to form “High‐entropy” perovskite NCs. In addition, compared with Cs(Pb0.72Mn0.14Ni0.14)Br3 NCs, Cs(Pb1/3Mn1/3Ni1/3)Br3 NCs have greater luminous intensity and stability, which because of the enhancement of band gap and valence bonds. Furthermore, photoluminescence intensity at 515 nm increase obviously when Cs(Pb1/3Mn1/3Ni1/3)Br3 NCs are heated at 120 °C. This is due to the lattice distortion effect brought about by ion doping. This study is expected to provide an effective way for synthesis and stability of all‐inorganic perovskite NCs doped with more kinds of different ions. Moreover, it also lays the foundation for the introduction of “High‐entropy” into perovskite functional ceramics.
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