‘Range anxiety’ is still the main problem for electric vehicles (EVs) to compete with the internal combustion engine vehicles. Ni-rich layered oxides (NLO) are deemed as one of the most promising cathodes for EVs because of their high capacity (>200 mAh g−1) above a charge of 4.3 V, relatively low cost, and environmental benignancy. Moreover, specific capacity of these layered oxide materials increases along with more Nickel content, up to a 240 mAhg−1 the limitation of LiNiO2. However, NLO compounds suffer several crucial problems like Li+/Ni2+ cation mixing, structural degradation, side reactions, and micro-cracks, which can accelerate the performance degradation of NLO cathodes. Just these problems hinder their application in Lithium-ion batteries (LIBs) for EVs. This project is to mitigate these problems of NLO based on innovative and effective coating and doping modification strategies, together with first-principle density functional theory (DFT) simulation study, to achieve higher power density, better rate capability, higher thermal stability, longer cycling life, and less cost NLO applied in advanced LIBs for EVs application.