Nanoparticles of a new dinuclear silver(I) complex [Ag2(PPh3)2(μ-S-4nb-tsc)2(η1-S-4nb-tsc)2](NO3)2, where 4nb-tsc = 4-nitrobenzylidenethiosemicarbazone and PPh3 = triphenylphosphine, were prepared in an ultrasonic bath and characterized by FT-IR and SEM. The crystal structure of a suitable single crystal prepared by slow evaporation was determined by single crystal X-ray diffraction. The compound crystallized in the triclinic system with space group P-1 and Z = 2. X-ray results showed that the neutral thiosemicarbazone ligand 4nb-tsc was coordinated to silver(I) ion in two different bonding modes, μ-S, and η1-S. The shortest distance between the sulfur-bridged Ag cations was 3.576(5) Å. One P atom and three S atoms from three 4nb-tsc ligands coordinated to the silver(I) ion in a distorted tetrahedral geometry. In the crystal packing of the title compound, several hydrogen bonds were connecting the molecules of the complex.