The global electrophilicity index (GEI) has been further explored as a general and base-free metric for Lewis acidity. A number of computational methods, including post-Hartree Fock, density functional theory, and time-dependent density functional theory, have been explored. In this fashion, we sought the method most applicable to a range of different Lewis acids with differing structural and electronic features, including boron trihalides, silicon tetrahalides, fluoroaryl boranes, and group 15 pentahalides. The most accurate and computationally efficient approach was found to use the energies of the orbitals from a geometry optimization at the B3LYP/def2-TZVP level of theory. In addition, the GEI is shown to act as an effective acidity metric that is complementary to the fluoride ion affinity. The GEI also proved to be a better gauge of Lewis acidity for softer bases, as confirmed by comparison to the iodide ion affinity of the group 15 pentahalides.