Layered double hydroxides (Ti-Al LDHs) with varying Ti/Al molar ratios were fabricated as adsorbents via the co-precipitation method, employing aluminum chloride, titanium chloride, and sodium hydroxide as raw materials. The influence of the composites on the F- adsorption performance under diverse conditions was examined. The Ti-Al LDHs and the recovered products after the reaction were characterized by SEM, BET, and XRD. The results indicated that the Ti-Al LDHs were more stable, exhibited a uniform stacking of the layer-like structure, and predominantly existed in a dispersed amorphous form with a wide pore size and a large specific surface area (108.34 m2/g). The experimental findings demonstrated that the maximum adsorption capacity reached 47.78 mg/g under the conditions of a dosage of 0.2 g/L, pH = 4, and a temperature of 35 ℃. The adsorption of fluoride by Ti-Al LDHs was more in line with the proposed second-order model (R2 > 0.99), and the adsorption isotherm was more consistent with the Langmuir model. After five adsorption-desorption cycles, the adsorption capacity was still equivalent to 73% of the initial capacity, presenting good regeneration performance. Ion exchange occurred between F and hydroxyl groups on the surface of Ti-Al LDHs, and the adsorption process was mainly attributed to ion exchange, electrostatic attraction and surface complexation.