By an easy co-precipitation method, the magnetic magnesium-aluminum-lanthanum composite was successfully synthesized. The effects of the synthetic conditions such as Mg/Al/La molar ratio and calcination temperature on fluoride removal by the adsorbent were studied. The adsorbents were characterized by scanning electron microscopy (SEM), X-ray diffraction (XRD), Fourier transform infrared (FT-IR) and energy-dispersive X-ray spectroscopy (EDS). By means of changing various conditions, such as contact time, solution pH, initial fluoride concentration, temperature and coexisting anions, batch adsorption studies were worked out. Results indicated that with a Mg/Al/La molar ratio of 16:1:1, at 500°C, near neutral pH and room temperature, the adsorbent obtained the maximum capacity of 65.75 mg/g for fluoride adsorption. The adsorption process was fitted well with the Langmuir isotherm model and the pseudo-first order kinetic model. Adsorption mechanism involved electrostatic interaction on surface and ion exchange interaction. All results indicated that the magnetic magnesium-aluminum-lanthanum composite can be a very promising adsorbent, has potential application in fluoride removal in water treatment and has positive effects on human health.