Semiempirical quantum mechanical (SEQM) methods offer an attractive middle ground between fully ab initio quantum chemistry and force-field simulations, allowing for a quantum mechanical treatment of the system at a relatively low computational cost. However, SEQM methods have not been frequently utilized in the study of transition metal systems, mostly due to the difficulty in obtaining reliable parameters. This paper examines the accuracy of the PM6 and PM7 semiempirical methods to predict geometries, ionization potentials, and HOMO-LUMO energy gaps of several bare gold clusters (Au-n) and thiolate-protected gold nanoclusters (AuSNCs). Contrary to PM6, the PM7 method can predict qualitatively correct geometries and ionization potentials when compared to DFT. PM6 fails to predict the characteristic gold core and gold-sulfur ligand shell (staple motifs) of the AuSNC structures. Both the PM6 and PM7 methods overestimate the HOMO-LUMO gaps. Overall, PM7 provides a more accurate description of bare gold and gold-thiolate nanoclusters than PM6. Nevertheless, refining the gold parameters could help achieve better quantitative accuracy.