We have studied theoretically the organometallic compound (NBu4)2[Au(3,5-C6F3Cl2)2Ag4(CF3CO2)5], whose dianionic part displays a AuAg4 square pyramidal arrangement based on closed-shell Au(I)...Ag(I) interactions between two monoanionic fragments. DFT/B3LYP, ab initio Hartree-Fock (HF), and second-order Møller Plesset perturbation theory (MP2) calculations have been carried out for simplified model systems. Model system [AuPh2]-...[Ag4(CO2H)5]- (C1) has been chosen from DFT results as an appropriate model for the study of the interactions. The four Au(I)...Ag(I) interactions and two additional C...Ag(I) interactions are observed when dispersion-type interactions are considered in the level of theory (MP2) displaying a metallophilic attraction between two anionic units. The study of model C2 (similar to C1 but with minimized C...Ag(I) interactions) permits the study of the Au(I)...Ag(I) interactions separately, which confirms the existence of stabilizing Au(I)...Ag(I) interactions around 13 kJ.mol(-1) each.