Application of aluminum substitution (doping) for transition metals are commonly used in lithium ion batteries to improve electrochemical performance, chemical and thermal stability of the cathode materials. However understanding the nature of surface and lattice aluminum environments or understanding possible aluminum diffusion on the interphase have been a challenge for aluminum bearing Li-ion battery materials such as LiNi1-y-zCoyAlzO2 (NCA), aluminum doped LiNixMnyCozO2 (NMC) and coated layered metal oxides. Solid state NMR spectroscopy is one of the few structural probes available that can qualitatively and quantitatively characterize lattice and non-lattice (i.e. surface, coatings, segregation, secondary phase etc.) aluminum coordinations. In the present study, we use NMR to gain new insights into transition metal (TM)-O-Al coordination’s, interfacial composition in pristine cathodes and evolution of lattice aluminum sites and solid electrolyte interface upon cycling. For each cathode composition, aluminum coordination of paramagnetic (lattice) and diamagnetic (non-lattice) nature have been investigated and their effect on cycling performance and surface film composition is reported.