The invention discloses a low-temperature hydrogen purification device which comprises a catalytic deoxidization device, a normal-temperature adsorption device, a low-temperature heat exchange device and a low-temperature adsorption device. Deoxidization is performed on crude hydrogen by the catalytic deoxidization device, the crude hydrogen is cooled to reach normal temperature by the catalytic deoxidization device, the normal-temperature adsorption device is used for adsorbing nitrogen in the crude hydrogen, the low-temperature heat exchange device is used for cooling the crude hydrogen, and the low-temperature adsorption device is used for adsorbing the nitrogen in the crude hydrogen. A gas inlet of the catalytic deoxidization device is connected with the crude hydrogen, a gas outlet of the catalytic deoxidization device is sequentially connected with the normal-temperature adsorption device, the low-temperature heat exchange device and the low-temperature adsorption device through pipelines, the normal-temperature adsorption device further can adsorb water and carbon dioxide in the crude hydrogen, and the low-temperature adsorption device further can adsorb micro-oxygen in the crude hydrogen. The invention further discloses a control method of the low-temperature hydrogen purification device. The low-temperature hydrogen purification device can obtain hydrogen with higher purity and better quality by the aid of tertiary purification technology, and the purification device further has the advantages of low operating cost, less equipment investment, convenience in operation, simplicity and convenience in maintenance and high reliability.