In this paper, copper oxide/covalent organic framework (CuO/COF) composites were prepared and investigated the photocatalytic performances for the removal of dyes. The characterization results of FTIR, XRD, and XPS, all proved that the CuO/COF composite were successfully prepared. The mapping of CuO/COF showed that the Cu element was uniformly distributed in the COF. After CuO was composited with COF, the energy band gap Eg decreased from 1.14 eV to 0.81 eV. The highest photocatalytic degradation rate of the CuO/COF composite was 94.00%. At the same time, the photocatalytic wavelength could be shifted from 254 nm to 356 nm. The enhancement of the photocatalytic activity of the CuO/COF composite was attributed to the increase in carrier transfer rate and the increase in the active sites. These results show that the CuO/COF photocatalyst has a strong potential for removing organic dyes under light of 254–356 nm, which also provides a certain reference value for the development of photocatalytic materials.