Here, we report the synthesis and experimental and theoretical characterizations of Au 36−x Ag x (SPh-tBu) 24 alloy nanomolecule to atomic precision. By changing the incoming gold-to-silver metal ratio during the synthesis of crude mixture, up to eight silver atoms can be incorporated into Au 36 (SPh-tBu) 24 , as theoretically confirmed and rationalized in terms of its core and staple structure. Tuning of optical response by Ag doping is strongly affected by aromatic conjugation and qualitatively different with respect to the aliphatic case, with a strikingly nonmonotonic behavior of absorption intensity in the low-and high-energy regions, in fair agreement with theoretical predictions, as rationalized via an original analysis tool: independent component mapping of oscillatory strength plots.