We report a new method for the processing of fly ash (FA) stabilized hydrogen titanate nano-sheets in the form of aggregated microspheres. The industrial silica-based FA has been utilized for this purpose which has been surface-modified by coating with the anatase-titania (TiO2) via sol-gel. The anatase-TiO2 coated FA particles are subjected to the hydrothermal treatment in an autoclave under high temperature and pressure conditions in a highly alkaline solution. The hydrothermal conditions cause dissolution of silica resulting in the disintegration of other constituents of FA which are adsorbed in ionic and/or oxidized form on the surface of intermediate product of the hydrothermal treatment of anatase-TiO2, specifically the hydrogen titanate. The adsorption of FA constituents has resulted in the stabilization of hydrogen titanate in the nano-sheet morphology instead of nanotubes. The FA stabilized hydrogen titanate nano-sheets exhibit higher specific surface-area than that of the hydrogen titanate nanotubes and have been successfully utilized for the removal of an organic synthetic-dye from an aqueous solution via surface-adsorption, involving the electrostatic-attraction and ion-exchange mechanisms operating, in the dark-condition. (C) 2012 Elsevier B.V. All rights reserved.