Abstract The crystal plane plays a very important role in the properties of Ni‐rich cathodes. [003] crystallographic texture regulation has been proven to improve structural stability, and yet, the discrepancy of particles with different exposed ratios of [003] in structural attenuation has not been clarified. Herein, we have unraveled comprehensively the structural decay difference for Ni‐rich cathodes’ primary particles with the different percentages of exposed [003] by regulating the precursor coprecipitation process. The findings based on structural characterization, first‐principles calculations, finite element analysis, and electrochemical test reveal that the length and width of particles represent [11¯0] $[1ar{1}0]$ and [003] directions, respectively, and show that cathode particles with a higher [11¯0] $[1ar{1}0]$/[003] ratio can effectively inhibit structure degradation and intergranular/intragranular crack formation owing to the low oxygen vacancy formation energy on (003) planes and the small local stress on secondary/primary particles. This study may provide guidance for the structural design of layered cathodes.
