The invention provides an adsorption-hydration reaction dual hydrogen-storing method and a device for realizing the hydrogen-storing method. The method provided by the invention comprises the following steps: 1) performing hydrophilic treatment on a carbon nanotube after the carbon nanotube is purified; 2) preparing a solution for generating hydrate, and uniformly spraying the prepared solution into the carbon nanotube treated in the step (1); 3) placing a mixed system of the soaked carbon nanotube and water solution into a hydrogen-storing tank, compacting the mixed system, covering a hydrogen-storing tank cover, sealing and standing by till uniformly mixing; and 4) vacuumizing the hydrogen-storing tank, and then connecting the hydrogen-storing tank with a hydrogen source, and performing a hydrogen-storing process. The device provided by the invention is mainly composed of the hydrogen-storing tank, the hydrogen source, a gas booster pump, a pressure instrument, a temperature observing system, a pipeline, and the like. The present problems of utilizing, storing and transporting hydrogen are solved according to the method and the device provided by the invention, the hydrogen storage rate is increased and the operation is convenient.