A new type of nano-adsorbent zinc-silver nanoparticles ornamented by multi-walled carbon nanotubes (Zn-Ag MWCNT) was efficiently synthesized by double arc discharge using a newly designed rotating cylinder electrode. Zn-Ag MWCNT was characterized by different instrumental methods to get information about the sample shape, size, and crystallinity. Without irradiation, Zn-Ag MWCNT indicated significant potential for elimination against methylene blue (MB) which is dissolved in deionized water. When the adsorbent concentration was 0.1 g/L at normal 8 pH, the Zn-Ag MWCNTs were efficient in removing 97% of the MB from 40 mg/L that was dissolved in water for 10 min. The dye removal activity of (Zn-Ag) decorated MWCNTs was attributed to the influence of silver and zinc nanoparticles on the MWCNTs. Finally, this approach was both cost-effective and efficient.