Photodegradation has been considered one of the most promising ways to treat wastewater. In this work, TiO2 (001)/Graphene Oxide (GO) nanocomposite has been successfully synthesized using hydrogen fluoride as a crystal-directing agent towards (001) facets. The nanocomposite was characterized by FTIR, XRD, Raman, HR-TEM, and diffuse reflectance spectra (DRS). Based on the result, the TiO2 (001) was decorated on the surface of the GO sheet with high absorption of visible light. In addition, as-prepared TiO2 (001)/GO nanocomposite provides a synergistic effect by increasing dye degradation activity with 95% and 99% removal rates for the photodegradation of methylene blue and crystal violet dyes, respectively, under LED irradiation for 10 min. The photodegradation kinetics of TiO2 (001)/GO was also successfully modeled and was found to follow the pseudo-first order kinetic. The enhanced photodegradation of the TiO2 (001)/GO nanocomposite attributed to the excellent synergy between TiO2 (001) nanoparticles and GO, which results in the highly efficient photocatalyst for removing organic pollutants in water.