Via a one-step ultrasonication method, cellulose nanofibril/graphene oxide hybrid (GO-CNF) aerogel was successfully prepared. The as-prepared GO-CNF possessed interconnected 3D network microstructure based on GO nanosheets grown along CNF through hydrogen bonds. The aerogel exhibited superior adsorption capacity toward four kinds of antibiotics. The removal percentages (R%) of these antibiotics were 81.5%, 79.5%, 79.1%, and 73.9% for Doxycycline (DXC), Chlortetracycline (CTC), Oxytetracycline (OTC), and tetracycline (TC), respectively. Simultaneously, the adsorption isotherms were well fitted to Langmuir model and kinetics study implied that the adsorption process was attributed to pseudo-second-order model. The maximum theoretical adsorption capacities of GO-CNF were 469.7, 396.5, 386.5, and 343.8 mg·g−1 for DXC, CTC, OTC, and TC, respectively, calculated by the Langmuir isotherm models. After five cycles, importantly, the regenerated aerogels still could be used with little degradation of adsorption property. Consequently, the as-synthesized GO-CNF was a successful application of effective removal of antibiotics.