Porous Al doped ZnO (AZO) nanosheets have been prepared as an efficient multifunctional water treatment material. Their fundamental properties were characterized by various spectroscopic testing methods. The AZO nanosheets displayed very rapid adsorption rate and high adsorption capacity for methyl orange (MO) dye. The kinetics and equilibrium of adsorption process were found to follow the pseudo-second-order kinetic and Langmuir isotherm models, respectively. Furthermore, the AZO nanosheets exhibited superior photodecolorizative activity compared with the commercial P25 TiO₂ nanoparticles. It was found that Al doping increased the zeta potential of AZO nanosheets and then significantly enhanced the adsorption capacity for MO dye and, at the same time, retarded the recombination of photoexcited electron–hole pairs, and prolonged the lifetime of the photo-generated carriers, and then improved the semiconductor photocatalytic activity. In addition, the visible-light-driven dye photosensitized degradation was also an important reason for enhanced photodecolorizative activity. Therefore, AZO nanosheets are a potential multifunctional water treatment material combining highly efficient adsorption and photocatalytic degradation.