density and long service life. General electromobility, which is considered necessary for the reduction of carbon emissions, requires the current EV market to grow exponentially; however, EV technology is confronted with significant performance and economic challenges, such as, limited driving range and battery durability and high battery costs, respectively. [1][2][3] These issues are directly related to the limitations of the LIBs powering EVs. Hence, improvements in the energy density and cycling stability of LIBs, as well as cost reduction, are prerequisites for envisioned general electromobility. Efforts have focused on developing high-capacity cathode materials because the overall performance of current LIBs is dictated by their cathodes. The capacity and cycle life of cathodes are generally inferior to those of graphite anodes (e.g., Li[Ni 0.8 Co 0.15 Al 0.05 ] O 2 and graphite have capacities of 200 and 360 mAh g -1 , respectively). Among the viable cathode materials for LIBs, layered Ni-rich lithium-nickel-cobalt-aluminum oxides, Li[Ni x Co y Al z ]O 2 (NCA), are the most promising materials for EV LIBs owing to their high theoretical capacity (278 mAh g -1 ) and good rate performance. [4,5] Recently, Tesla Motors adopted NCA materials in LIBs to power their Models S, X, and 3, which are capable of operating for 400-550 km per single full charge. However, to compete against internal combustion engine vehicles, EVs should have a driving range exceeding 600 km per single charge, which can be achieved by increasing the energy density of the cathode. Increasing the energy density of an NCA cathode requires increasing its relative fraction of Ni. [6] However, a highly delithiated NCA cathode, when charged to 4.3 V, suffers from structural degradation at the cathode particle surfaces owing to reaction between unstable Ni 4+ and the electrolyte that forms a deleterious NiOlike rock salt impurity phase. [7][8][9] Furthermore, Ni-rich layered cathodes (relative Ni fraction ≥ 0.8) undergo abrupt lattice contractions in the c-axis direction caused by H2→H3 phase transitions (at ≈4.15 V), which generate microcracks. [9][10][11][12][13][14][15] The severity of the microcracking increases with increasing Ni content. [14] The microcracks cause the electrolyte to penetrate the particle interior and attack inner primary particles, causing structural degradation, which leads to capacity fading and eventually to catastrophic mechanical failure. [6,7,[12][13][14][15] Moreover, this degradation triggers oxygen release from the host structure, giving riseThe Nb doping of Li[Ni 0.855 Co 0.13 Al 0.015 ]O 2 (NCA85) modifies its primary particle morphology to allow precise tailoring of its microstructure. The Nb dopant (1 mol%) elongates the primary particles and aligns them in the radial direction, creating a configuration that effectively dissipates the abrupt internal strain caused by H2↔H3 phase transitions near the charge end. The negation of the internal strain substantially improves the long-term cycling stability achieved...