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Ni‐rich cathodes with superior energy densities have spurred extensive attention for lithium‐ion batteries (LIBs), whereas their commercialization is hampered by structural degradation, thermal runaway, and dramatic capacity fading. Herein, boron (B) with high binding energy to oxygen (O) is gradiently incorporated into each primary particle and piezoelectric Li2B4O7 (LBO) is homogeneously deposited...