To make full use of natural waste, a novel Mg-Al mixed oxide adsorbent was synthesized by the dip-calcination method using the fluff of the chinar tree (FCT) and an Mg(II) and Al(III) chloride solution as raw materials. The adsorbents were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), Fourier transform infrared (FT-IR) spectroscopy, and X-ray photoelectron spectroscopy (XPS). The effects of the Mg/Al molar ratio and calcination temperature on the performance of the novel Mg-Al mixed oxide adsorbent were investigated. The optimized Mg-Al mixed oxide adsorbent had a Langmuir adsorption capacity of 53 mg/g. This adsorption capacity was higher than that of the separate Mg oxide and Al oxide. The synergy between Mg and Al is beneficial to the adsorption performance of the material. The fluoride adsorption capacity of the optimized Mg-Al mixed oxide adsorbent is only slightly affected by ions such as Cl−, NO3−, SO42−, Na+, and K+ and is excellent for use in recycling and real water. The hydroxyl groups on the surface of the Mg-Al mixed oxide adsorbent play a key role in the adsorption of fluorine. The as-obtained novel Mg-Al mixed oxide adsorbent is an efficient and environmentally friendly agent for fluoride removal from drinking water.