By studying the correlation between experimentally measured Al NMR parameters and DFT calculated results with a relatively large benchmarking set, we can confirm that DFT calculation is accurate in predicting isotropic chemical shift δ iso and quadrupolar coupling constant C Q for crystalline materials that contain Al. The same as our previous benchmarking effort on spin ½ nuclei Si, DFT prediction on asymmetry parameters (both η CS and η Q ) is shown to be more prone to error due to the sensitivity of this parameter to slight variation in local geometry and the difficulty of accurately measure η experimentally.