Layered LiNi1/3Mn1/3Co1/3O2 (NMC) positive materials were synthesized by efficient, low-cost, and easily manageable methods such as oxalate co-precipitation and sol-gel processes. Preliminary electrochemical results show that sol-gel samples provide better results than co-precipitated samples.With the aim of improving the properties of the co-precipitated samples, these were coated with carbon and alumina, considering the co-precipitation method’s suitability for large-scale production. The subsequently performed local structure investigations revealed well-crystallized layered cathode materials with an αNaFeO2-type structure (R-3m space group).Sample tests using both the scanning electron microscope (SEM) and the transmission electron microscope (TEM) showed submicron particles with a slight tendency to agglomerate and the existence of a thin film encapsulating the oxide particles. 7Li magic angle spinning nuclear magnetic resonance (7Li MAS NMR) measurements were carried out for pristine and coated samples to compare the cation arrangement in the transition metal layers.Finally, electrochemical tests revealed a remarkable improvement in capacity retention of the coated oxides compared to the parent compounds.