To overcome the hard and costly post-treatment separation of ultrathin graphitic carbon nitride nanosheets (UGCN), it was supported on polyurethane foam (PUF). The ratio of PUF/UGCN was optimized for the removal of a mixture of methylene blue (MB) and methyl orange (MO) dyes. The characteristics of the composite photocatalyst and its photocatalytic performance were detailly studied. The X-ray diffraction and Fourier transform infrared results proved the successful preparation of UGCN and PUF and that the PUF/UGCN composite combines the features of both pure materials. The transmission electron microscopy illustrated the ultrathin nanosheet shape of the UGCN, while the scanning electron microscope showed the highly porous 3D-hierarchical structure of PUF. Compared to the pure components, the composite photocatalyst with PUF/UGCN mass ratio of 4 achieved better decolorization of MO and almost same decolorization of MB as UGCN. Neutral pH and 1 g/L of the composite photocatalyst were the optimum conditions for MB/MO mixture decolorization. The composite photocatalyst kept its efficiency for five successive cycles. Hydroxyl radicals were the dominant in the degradation of MB, while superoxide radicals were the most influencer in MO degradation. Conclusively, supporting UGCN onto PUF kept the photocatalytic efficiency of UGCN toward MB decolorization and improved its efficiency toward MO. Moreover, it enabled the reuse of the composite photocatalyst and facilitated the post-treatment separation process.