Development of new adsorbent based on anionic silica precursor, cellulose nanofiber (CNF), and graphene oxide (GO) has prepared via ionic reaction followed by a sol-gel process. Different instruments were used for the characterization of the nanocomposite: Fourier transform infrared spectrometer (FTIR), X-ray diffraction (XRD), scanning electronic microscope (SEM), Thermal gravimetric analysis (TGA), and transmission electron microscope (TEM). Methylene blue (MB) adsorption on CNF/GO and CNF/GO/silica nanocomposites achieved during 60 min. A pseudo-second-order kinetic model was fitted to the adsorption process, with a maximum adsorption capacity of 588.23 and 625 mg/g in a slightly alkaline solution, respectively. It was found that the adsorption capacity of CNF/GO and CNF/GO/silica could regenerate the MB up to four cycles with slight decrease from 98 to 93%. This study showed that CNF/GO and CNF/GO/silica nanocomposites are effective adsorbents for organic pollutants in wastewater.