Adsorption materials play very important roles when used to effectively remove organic pollutants from the environment. In this paper, a novel graphene oxide/COFs (GO/COFs) composite was synthesized by the Schiff base coupling reaction between 1,3,5-tri(4-aminophenyl)benzene and 2,5-divinylterephthalaldehyde on the surface and between layers of GO at room temperature. The synthesized GO/COFs composite has a low density, large specific surface area, layered porous structure and favorable water dispersion. The adsorption behavior of the GO/COFs composite for naphthalene, 1-naphthylamine and 1-naphthol in aqueous solution was studied. Compared with GO and the COFs alone, the composite has a higher adsorption capacity, which may be due to the synergistic effect of the COFs and GO. In addition, the GO/COFs composite achieves excellent regeneration capability through ultrasound in ethanol, which is a low energy consumption and easy to operate method. This composite is hoped to be an excellent adsorbent in environmental remediation.