Capacitive deionization, as a second generation electrosorption technique to obtain water, is one of the most promising water desalination technologies. Yet; in order to achieve high CDI performance, a well-designed structure of the electrode materials is needed, and is in high demand. Here, a novel composite nitrogen-TiO2/ZrO2 nanofibers incorporated activated carbon (NACTZ) is synthesized for the first time with enhanced desalination efficiency as well as disinfection performance towards brackish water. Nitrogen and TiO2/ZrO2 nanofibers are used as the support of activated carbon to improve its low capacitance and hydrophobicity, which had dramatically limited its adequacy during the CDI process. Importantly, the as-fabricated NACTZ nanocomposite demonstrates enhanced electrochemical performance with significant specific capacitance of 691.78 F g−1, low internal resistance and good cycling stability. In addition, it offers a high capacitive deionization performance of NACTZ yield with electrosorptive capacity of 3.98 mg g−1, and, good antibacterial effects as well. This work will provide an effective solution for developing highly performance and low-cost design for CDI electrode materials.