Water treatment for the removal of organic or inorganic pollutants has become a serious global issue because of the increasing demand for public health awareness and environmental quality. The current paper, reports the applicability of mesoporous aluminosilica monoliths with three-dimensional structures and aluminum contents with 19 <= Si/Al >= 1 as effective adsorbents of organic molecules from an aqueous solution. Mesocage cubic Pm3n aluminosilica monoliths were successfully fabricated using a simple, reproducible, and direct synthesis. The acidity of the monoliths significantly increased with increasing amounts of aluminum species in the silica pore framework walls. The batch adsorption of the organic pollutants onto (10 g/L) aluminosilica monoliths was performed in an aqueous solution at various temperatures. These adsorbents exhibit efficient removal of organic pollutants (e.g., aniline, p-chloroaniline, o-aminophenol, and p-nitroaniline) of up to 90% within a short period (in the order of minutes). In terms of proximity adsorption, the functional acid sites and the condensed and rigid monoliths with tunable periodic scaffolds of the cubic mesocages are useful in providing easy-to-use removal assays for organic compounds and reusable adsorbents without any mesostructural damage, even under chemical treatment for a number of repeated cycles. (C) 2011 Elsevier B.V. All rights reserved.