Layered double hydroxides (LDHs) are limited by a lack of adsorption active sites and low porosity, leading to a suboptimal performance in antibiotic adsorption. In this study, LDH was used as templates to obtain LDO through high-temperature calcination, creating rapid mass transfer channels for LVX, thereby enhancing adsorption capacity and reducing adsorption time. Subsequently, small ZIF-67 crystals were grown in situ between the layers and on the surface of LDOs, providing additional adsorption active sites and surface area to the LDO@ZIF-67 composite material. In the LVX removal process, the synergistic effect between LDO and ZIF-67 mainly depends on the "memory effect" and the interaction of various mechanisms such as metal complexation, hydrogen bonding, and electrostatic attraction. LDO@ZIF-67 exhibits a rapid adsorption rate toward LVX, reaching adsorption equilibrium within 40 min, with an adsorption capacity as high as 268 mg/g, surpassing values reported in some literature. The adsorption process was more consistent with the Langmuir (