In summary, we developed a facile approach to modify the NMC811 cathode structure by coating the surface with Al2O3 and MoO3, using a plasma-enhanced atomic layer deposition technique. According to the characterization analysis, homogenous layers of Al2O3 and MoO3 were deposited on the NMC811. In addition, the data attained from the XRD spectra, as well as the SAED examination, exhibited in-line results in terms of the crystalline structure of the prepared cathodes and the coating can reduce Li and Ni mixing, and stabilize the NMC811 crystal structure. The EIS data revealed that the boosted electrochemical performance through the coating step could be linked with a reduction in the impedance, the formation of a strengthened structure against HF, and the suppression of electrolyte decomposition reaction. An in-depth study of the electrochemical performance showed the enhancement of capacity retention through coating with Al2O3 and MoO3 layers. Taken together, the Al2O3 PEALD coated layer represented superior performances regarding ionic conductivity, charge/discharge reversibility, and capacity retention in comparison with the MoO3 protective layer. The obtained data suggest exploring alumina coating with superior Li-ion conductivity toward the growth and progress of NMC coating. Furthermore, the study of the designed coated structure in full cells is of value in this era.