The current study aims at combining two building blocks together into well-designed nanostructures to act as dual-function materials; active photocatalysts in sunlight and effective adsorbents for increasing the efficiency of water purification. By these nanostructures, we could avoid the drawbacks of the existing technologies for water purification and remove the industrial pollutants by a dual process; adsorption and photocatalytic degradation. In this trend, Zn-Al layered double hydroxides (LDHs) are combined with graphene oxide to produce a series of nanolayered structures. These nanolayered structures are effective for converting Zn-Al LDHs to be photo-active in sunlight through decreasing its band gap energy from 5.5 eV to 2.5 eV. In addition, these nanolayered structures caused complete decolorization and mineralization of green dyes in sunlight through accelerating the reaction rate of the photocatalytic degradation of dyes seven times higher than that of the pure Zn-Al LDHs. In the same time, they improved the adsorption process of green dyes through creating new micro- and meso-porous structures and high surface area for Zn-Al LDHs. Finally, the well-designed nanostructures between Zn-Al LDHs and graphene oxide led to converting non-photoactive materials to be active in the visible light in addition to a complete and fast removal for organic pollutants.