Nowadays, the energy supply market for commercial electrical vehicles and mobiles is highly dominated by Li-ion batteries (LIBs). The layered Li-rich (LLR) oxide MNC (Mn, Ni, and Co)-based cathode is a promising material for next-generation LIBs due to its high energy and power density, cost-effectiveness, and eco-friendliness. However, LLR material’s micrometer-size particles can lead to intergranular cracks during electrochemical cycling at high voltages, resulting in a thick solid electrolyte interphase. Along with this, structural fluctuations, particle agglomeration and non-uniform particles, oxygen loss in initial cycling, Mn dissolution, irreversible cation migration, high internal resistance, and corrosion contribute to issues like low charge–discharge capacities, voltage fade, irreversible capacity loss, poor Coulombic efficiency, and limited rate capability, degrading the electrochemical performance of the LLR cathode. Fortunately, the nanomaterials (NMs) coating, including oxides, phosphates, fluorides, carbon compounds, and polymers, offers solutions through core/shell strategies composed of LLR core and nanoscale shell. This article delves into NM coating advantages and methods for achieving uniform, homogeneous, and ultrathin nanocoatings (less than 40 nm thickness). Additionally, incorporating the ultrathin spinel layer and oxygen vacancies can further enhance the electrochemical activity.