A novel composite material (Zn/Cu-BTC@MC) composed of bimetallic Zn/Cu-BTC and mesoporous carbon (MC) has been successfully synthesized by one-pot hydrothermal reaction. We have approved that MC was successfully wrapped around the surface of Zn/Cu-BTC and the existence of the crystal state by various characterization methods. The Zn/Cu-BTC of this composite material is microporous while the MC is mesoporous, which is beneficial for Congo red (CR) to diffuse in the MC and adsorb in the Zn/Cu-BTC. Because of the excellent surface area and bimetallic synergistic effect, the Zn/Cu-BTC@MC exhibits a high uptake capacity and selectivity toward CR; this is even more outstanding than other adsorbents reported previously. In addition, the novel composite adsorbent possessed a good water resistance for CR capture from aqueous solution. Saturated adsorbent Zn/Cu-BTC@MC can be regenerated by solvent elution and nitrogen purging. Over 91% of the CR absorption capacity could be recovered with water molecules after regeneration. The distinctive structure of Zn/Cu-BTC@MC might be a hopeful adsorbent for anionic dye purification such as CR.