The Zr and B co-doped Ni-rich Li[Ni0.885Co0.100Al0.015]O2 cathode shows extraordinarily stable cycle performance. The Li[Ni0.885Co0.100Al0.015]O2 cathode doped with 0.3 mol% Zr and 1.5 mol% B exhibits remarkable long-term cycling by retaining 95% of its initial capacity even after 1000 cycles whereas the pristine Li[Ni0.885Co0.100Al0.015]O2 cathode retains only 62% after 500 cycles. The unprecedented stability performance of the co-doped Li[Ni0.885Co0.100Al0.015]O2 cathode is attributed to the microstructure modification that inhibits microcrack propagation in the deeply charged state. Although the proposed cathode may not be an ideal cathode for use in a high-end EV due to its inferior rate capability, the co-doped Li[Ni0.885Co0.100Al0.015]O2 is well suited for applications where power demand is moderate and battery life and cost are critical. Moreover, the proposed cathode suggests that appropriate microstructure modification can effectively resolve the inherent capacity fading of Ni-rich layered cathodes, providing the material design guidelines for the next generation of high-performance LIBs.