MWCNT/BiOBr composite was successfully designed through interfacial linkage of amide bonds or hydrogen bonds by utilizing the reaction between amino groups of MWCNT and residual carboxyl or hydroxyl groups on the surface of prepared BiOBr. Retaining similar morphology, size and crystallinity with pure BiOBr, the obviously enhanced photocatalytic performance of the 2 wt.% MWCNT/BiOBr composite can be attributed to effective capture and transport of photo-generated electrons by MWCNT through the interfacial covalent bond.