The invention belongs to the technical field of composite materials, and particularly relates to a zinc-aluminum hydrotalcite carbon nanotube composite adsorption material and a preparation method andapplication thereof. The preparation method comprises the following steps: adding carbon nanotubes into a three-neck round bottom flask filled with concentrated nitric acid and concentrated sulfuricacid, stirring and reacting in an ultrasonic water bath for 1.5h, cooling to room temperature, filtering by suction and washing, and drying to obtain an intermediate product named CNT-COOH; weighing zinc chloride and aluminum chloride hexahydrate in a beaker, adding deionized water, stirring to dissolve, adding the intermediate product obtained in the step 1), slowly dropping a 2 mol L<-1> NaOH solution at a certain speed, adjusting pH to 10, stirring for 2-5 hours, and carrying out hydrothermal reaction to obtain the target product, Zn/Al-LDH @ CNTs. The method has the advantages of low synthesis cost, simple synthesis method, energy conservation, environmental protection, large adsorption capacity, high adsorption speed, wide application and practical applicability.