Ag nanoparticles were distributed onto polystyrene nanoparticle (PS-Ag) beads using two synthetic methodologies. In the first methodology, polystyrene (PS) beads were prepared via emulsion polymerization, with Ag nanoparticles subsequently loaded onto the surface of the PS beads. The polymerization of styrene was radiolytically induced in an ethanol (EtOH)/water medium, generating PS beads. Subsequently, Ag nanoparticles were loaded onto the PS beads via the reduction of Ag ions. The results from the morphological studies, using field emission transmission electron microscopy (FE-TEM), reveal the PS particles were spherical and nanosized, and the average size of the PS spherical particles decreased with increasing volume % of water in the polymerization medium. The size of the PS spherical particles increases with increasing radiation dose for the polymerization. Also, the amount of Ag nanoparticle loading could be increased by increasing the irradiation dose for the reduction of the Ag ions. In the second methodology, the polymerization of styrene and reduction of Ag ions were simultaneously performed by irradiating a solution containing styrene and Ag ions in an EtOH/water medium. Interestingly, the Ag nanoparticles were preferentially homogeneously distributed within the PS particles (not on the surface of the PS particles). Thus, Ag nanoparticles were distributed onto the surface of the PS particles using the first approach, but into the PS clusters of the particles via the second. The antimicrobial efficiency of a cloth coated with the Ag-PS composite nanoparticles was tested against bacteria, such as Staphylococcus aureus and Klebsiella pneumoniase, for 100 water washing cycles.