Thiolate-stabilized gold nanoclusters have drawn significant attention for their extraordinary properties and their applications in many fields such as catalysis, sensing, biomedicine, etc. However, due to the size, complexity, and conformational flexibility of thiolate ligands, accurate structure prediction can be a challenge using computational approaches. Substitution of thiolate ligands with chloride ligands provides a possible alternative. In this work, the stabilities of a series of gold thiolate and chloride clusters with 1:1 stoichiometry (AunLn; L = SH, Cl; n = 2-9) and the analogs of some experimentally observed gold nanoclusters (AunLn; L = SH, Cl; n = 18-133) are examined, and binding energies, HOMO-LUMO gaps, and absorption spectra are determined using density functional theory (DFT). We observed that the optimized geometries of gold nanoclusters for both types of ligands converged to the same local minimum structure as the experimentally observed structures. The average binding energy per gold atom in gold clusters converges after Au4L4. The binding energies of chloride-stabilized gold clusters and nanoclusters average 87.5% and 95.7% of the binding energies of thiolate-stabilized systems for the clusters and nanoclusters, respectively. Typically, thiolates are found to be more stable than the chlorides. However, higher HOMO-LUMO gaps in Au2Cl2, Au38Cl24, and Au102Cl44 compared to their thiolate analogs suggest systems of particular interest for investigating the possible existence of chloride-based gold nanoclusters. Absorption spectra are very similar regardless of the ligand used. This study also demonstrates that in theoretical studies on large nanoclusters, complex thiolate ligands can be replaced by Cl ligands to predict structural and electronic properties with reasonable accuracy and reduced computational effort.