Fluoride contamination in water is a key problem facing the world, leading to health problems such as dental and skeletal fluorosis. So, we used low-cost multifunctional tea biochar (TBC) and magnetic tea biochar (MTBC) prepared by facile one-step pyrolysis of waste tea leaves. The TBC and MTBC were characterized by XRD, SEM, FTIR, and VSM. Both TBC and MTBC contain high carbon contents of 63.45 and 63.75%, respectively. The surface area of MTBC (115.65 m²/g) was higher than TBC (81.64 m²/g). The modified biochar MTBC was further used to remediate the fluoride-contaminated water. The fluoride adsorption testing was conducted using the batch method at 298, 308, and 318 K. The maximum fluoride removal efficiency (E%) using MTBC was 98% when the adsorbent dosage was 0.5 g/L and the fluoride concentration was 50 mg/L. The experiment data for fluoride adsorption on MTBC best fit the pseudo 2nd order, rather than the pseudo 1st order. In addition, the intraparticle diffusion model predicts the boundary diffusion. Langmuir, Freundlich, Temkin, and Dubnin–Radushkevich isotherm models were fitted to explain the fluoride adsorption on MTBC. The Langmuir adsorption capacity of MTBC = 18.78 mg/g was recorded at 298 K and decreased as the temperature increased. The MTBC biochar was reused in ten cycles, and the E% was still 85%. The obtained biochar with a large pore size and high removal efficiency may be an effective and low-cost adsorbent for treating fluoride-containing water.