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A novel aluminium oxy hydroxide [Al–O(OH)] modified graphene oxide was prepared by a chemical precipitation method wherein Al3+ ions could interact effectively with the different functional groups of graphene oxide (GO). The prepared (GO–Al–O(OH) adsorbent was tested for the effective defluoridation of water. The Al3+ modified graphene oxide adsorbent was characterized using FT-IR, FT-Raman, SEM-EDS, XRD and XPS studies. The thermodynamically feasible adsorption is supported by the pseudo second order kinetics and a high Langmuir maximum adsorption capacity (51.42 mg g−1) for the GO–Al–O(OH) adsorbent. Furthermore, we could treat 2.0 L of 5.0 mg L−1 fluoride ion solution to bring the level within the permissible limits and the regeneration of the adsorbent was done using ammonium hydroxide.