A new synthetic route for decorating carbon nanotubes (MWCNTs) with silver nanoparticles by proton beam irradiation at room temperature is presented. Pristine- and surface-modified MWCNTs were comparatively utilized for the preparation of MWCNT-Ag-nanoparticles nanohybrid. Silver nanoparticles on the surfaces of MWCNTs were produced in situ without any additional reducing reagents, and more importantly, all the solutions were aqueous phase-based. The surfaces of MWCNTs were functionalized with thiol groups using several steps, which included an oxidation step. The silver nanocrystals on the surface-modified MWCNTs were spherical and -4 nm in diameter. Thiolated MWCNTs were well decorated with Ag nanoparticles, whereas pristine MWCNTs were not.