Titanium carburizing electrodes were used as the electrodes in a capacitive deionization (CDI) process for desalination in this study. Two methods of high vacuum magnetron sputtering and chemical deposition were used for the preparation of nano-titanium carburizing electrodes (named Ti-C* and Ti-C**). By comparing the adsorption capacities of different kinds of electrode material, combined with physical and chemical characteristics and electrochemical analysis, the method of high vacuum magnetron sputtering to prepare Ti-C* electrodes have been proved successful for the CDI process. The results show that under the same conditions, the adsorption capacity of Ti-C* and Ti-C**were 9.6 mg/g and 7.12 mg/g, respectively. The Ti-C* electrodes showed a higher ion electrosorption capacity than Ti-C** and the electrodes can be easily regenerated, indicating excellent recyclability. This study provided a novel method to fabricate titanium carburizing electrodes in CDI process and might lead to the improvement of the CDI desalination performance in an industrial practical application.