Porous gamma-Al2O3 material with viable morphologies and structures were prepared via a facile surfactant-assisted hydrothermal synthesis followed by calcination. The characterization results indicate that the mesoporous gamma-Al2O3 with hierarchical nanoarchitectures are composed of nanosized aluminium oxide crystallites as building units and possess high surface area (maximum of 164.27 m(2)/g with assistance of sodium dodecyl sulfate (SOS)). Depending on different surfactants as the crystallization modifiers, the gamma-Al2O3 exhibited various morphologies, such as flowerlike aggregation of nanosheets, spindles of twisted nanoflakes, or thinner featherlike particles. Using parachlorophenol as model pollutant, the batch adsorption experiments were carried out in order to investigate the adsorption capacity of the prepared materials. It was revealed that pseudo-second-order kinetic model can better describe the adsorption kinetics. Furthermore, the equilibrium adsorption data were congruous with the Jovanovic model with maximum adsorption capacity of 163.1 mg/g. The as-prepared Al2O3 materials with hierarchical pore structure and specific surface area would be regarded as effective adsorbents for the removal of parachlorophenol in water.