An ab initio one-pot synthesis of the bimetallic clusters [AunAg44-n (SC6H3F2)(30)](4-) (abbreviated (AuAg)(44); n <= 12) is reported. The mixed-metal (AuAg)(44) clusters, synthesized with different reactant Au/Ag ratios, exhibit a fractal-like distribution, suggesting that nucleation of the icosahedral core is a fractal growth process. X-ray crystallographic studies provided unambiguous evidence that the doped Au atoms occupy the icosahedral sites and the maximal doping is 12. The number of Au atoms (n) in [AunAg44-n(SR)(30)](4-) (SR = SC6H3F2) can be continuously tuned from 0 to 12. A three-way correspondence between single-crystal structure, MS, and UV-vis is established, thereby facilitating future identification (finger-printing) of the alloy [Au6Ag44-n(SR)(30)](4-) clusters. The temperature, solvent, and temporal effects in the synthesis were also investigated.