Cobalt-based materials are reported to be the most efficient catalysts in sulfate radical advanced oxidation processes (SR-AOPs). A green and facile method was developed in this work to prepare uniform Co(OH)2 hexagonal nanosheets, which was void of any organic solvents via mere ambient temperature stirring. The obtained nanosheets were assembled into a catalytic gravity-driven membrane, through which the removal efficiency of a typical pharmaceutical contaminant, ranitidine (RNTD), could reach ∼100% within 20 min. Meanwhile, the catalytic membrane also demonstrated effective removal performance towards various pollutants. In order to augment the long-term stability of catalytic membranes, Co(OH)2/rGO composites were fabricated using the same strategy, and a Co(OH)2/rGO catalytic membrane was prepared correspondingly. The Co(OH)2/rGO membrane could maintain a ∼100% removal of RNTD over a constant reaction period lasting for up to 165 hours, which was approximately 11 times that of the sole Co(OH)2 membrane (15 h). Analysis of element chemical states, metal ion concentration in filtrates, and quenching experiments suggested that the combination with rGO could promote the electron transfer to accelerate the Co(II) regeneration, restrain the cobalt dissolution to alleviate the active site loss, and contribute to the production of 1O2via synergistic effects of oxygen-containing groups in rGO. Toxicity assessment was performed on RNTD and its degradation intermediates to confirm the reduction in ecotoxicity of the treated feed. Overall, this work not only offered guidance for the application of nanosheets in AOP membranes, but also had implications for the environmentally-friendly preparation protocol to obtain functional metal hydroxides.