Three-dimensional (3D) ZnO nanorods with good adsorption property was successfully fabricated via a facile hydrothermal method, and characterized by scanning electron microscopy (SEM), X-ray diffraction (XRD), Energy Dispersive X-ray spectrometer (EDX) and a UV-vis spectrophotometer. It was found that the ZnO nanorods with a diameter of ~0.5 µm and the length of ~10 µm were firmly grown on the struts of the open-cell aluminum foams, and the 3D hierarchical structured adsorbent ZnO nanorods/Al foam (r-ZnO/AF) exhibits a higher adsorption capacity for Brilliant Blue R (BBR) in aqueous solutions, more stable sorption regenerable behavior and solid–liquid separability in contrast to the corresponding n-ZnO powder sample. The kinetics of the adsorption process was also discussed.