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A novel natural phosphate/graphene oxide (GO) composite membrane was successfully fabricated using two steps: (i) silane chemical grafting and (ii) dip-coating of a GO solution. First, the low-cost disk ceramic support used in this work was fabricated out of Moroccan natural phosphate, and its properties were thoroughly characterized. The optimized ceramic support was sintered at 1100 °C following a specific heat treatment based on thermogravimetric analysis (TGA) and differential thermal analysis (DTA); it exhibited a permeability of 953.33 L/h·m2·bar, a porosity of 24.55%, an average pore size of 2.45 μm and a flexural strength of 22.46 MPa. The morphology analysis using SEM showed that the GO layer was homogenously coated on the crack-free Moroccan phosphate support with a thickness of 2.8 μm. The Fourier transform infrared spectrometer (FT-IR) results showed that modification with silane could improve the interfacial adhesion between the GO membrane and the ceramic support. After coating with GO on the surface, the water permeability was reduced to 31.93 L/h·m2·bar (i.e., by a factor of 142). The prepared GO/ceramic composite membrane exhibited good efficiency in the rejection of a toxic azo dye Congo Red (CR) (95.2%) and for a simulated dye effluent (87.6%) under industrial conditions. The multi-cycle filtration tests showed that the rejection rate of CR dye remained almost the same for four cycles. Finally, the flux recovery was also studied. After 1 h of water cleaning, the permeate flux recovered, increased significantly, and then remained stable.