In this study, novel lamellar double hydroxide composites (LDH-MgAl and LDH-MgFe) were synthesized at different metal salt ratios (1:1 to 3:1) and fully characterized using various techniques such as XRD, FTIR, SEM, EDS, and TGA. The resulting LDHs demonstrated a high affinity for efficiently removing tetracycline (TC) antibiotic from water, particularly at a moderate molar ratio of 3:1. This ratio exhibited improved structural characteristics, resulting in better TC uptake from water. The improved performance was supported by the increased abundance of surface functional groups (OH, NO3, CO32-, C-O-C, Fe-O, and Al-O-Al). The TGA analysis established the high stability of the LDHs when subjected to high temperatures. The kinetics of TC adsorption onto LDH fitted with the PSO (R2 = 0.935-0.994) and Avrami (R2 = 0.9528-0.9824) models, while the equilibrium data fitted the Liu and Langmuir isotherm models, with maximum monolayer adsorption capacities of 101.1 mg g-1 and 70.83 mg g-1, respectively-significantly higher than many reported values in the literature. The positive values of ΔH0 and ΔS0 indicate an endothermic process, with TC removal mechanisms influenced by physical interactions, such as hydrogen bonding, electrostatic interaction, and π-cation with the surface functional groups of the LDH adsorbents. These results suggest that LDH-MgAl and LDH-MgFe are promising adsorbents for the removal of TC from water.