Excess fluoride in water can result in serious health problems. For this reason, we have developed a novel Ce-Zn binary metal oxide (Ce-Zn BMO) adsorbent for high-performance fluoride adsorption from drinking water. The Fourier transform infrared spectroscopy (FTIR) and X-ray photoelectron spectroscopy (XPS) results demonstrated both electrostatic interactions and ion exchange of surface hydroxyl groups of Ce-Zn BMO with fluoride ions. The Ce-Zn BMO adsorbent exhibited a good Langmuir adsorption capacity of 194 mg/g at pH 7.0. The adsorbent has a wide pH range (3-7) applicability and negligible coexisting ion effect that makes it an attractive sustainable material for field applications. Column adsorption studies indicated the efficient treatable volume as ∼94-bed volume (BV) using natural water when the breakthrough point in the column was 1.5 mg/L. Furthermore, six cycles reusability without much loss of adsorption capacity and effective column treatment of fluoride contaminated water indicated that Ce-Zn BMO could be developed into an efficient technology for high performance elevated fluoride water treatment.