It has been reported that the solid-state diffusivity can vary by several orders of magnitude between grain boundary (GB) diffusion and lattice diffusion in various solid-state systems . Recently, He et al. applied a first-principles theoretical approach to systematically study the Li diffusivity under different GB conditions in NMC cathode materials. In this work, we have adopted a similar atomistic approach to investigate Li diffusivity in LNMO cathode materials. The results are shown in Figure , in which Li-ion migration pathway across Σ3 (011) from site A to F is illustrated in (a), and the corresponding energy profiles for each step are plotted in (b). It is evident that Li ions need significantly less energy to migrate within GB (C to D) than within the bulk matrix (A to B, or E to F). Additionally, the two bulk-to-GB energy profiles (B to C and D to E) behave differently. The path of D to F, crossing Mn, presents a lower energy barrier than the path of B to C, which crosses Ni. Further investigations will be carried out to understand this interesting observation. In general, the computation results for LNMO are in line with other studies showing that GBs promote Li diffusivity. More GB conditions for LNMO are under investigation, and the comprehensive analysis will be reported elsewhere as an independent work.