In this study, a nitrogen and sulfur co-doped sodium titanium phosphate/hole graphene (N,S-NTP/rHGO) was synthesized by one-step hydrothermal method using thiourea as N/S source. The microstructure characterization confirms that N and S heteroatoms have been integrated into the graphene skeleton. The electrochemistry and electrosorption properties of the N,S-NTP/rHGO electrodes were investigated for hybrid capacitor deionization (HCDI). The results indicate that the specific capacitance of N,S-NTP/rHGO electrodes can reach 530.46 F g(-1) at a scan rate of 0.2 mV s(-1), which is 33.8% higher than that of the sample without doping. Moreover, the HCDI cell based on the N,S-NTP/rHGO-2 shows a high desalination capacity of 36.87 mg g(-1) and a rapid ion removal rate of 0.66 mg g(-1) s(-1), which is more than twice as high as the sample without doping (0.3 mg g(-1) s(-1)) at an initial NaCl concentration of 800 mg L-1 and applied voltage of 1.4 V. Further, the N,S-NTP/rHGO electrode exhibits excellent regeneration ability. Therefore, this study suggests that as-prepared N,S-NTP/rHGO composite exhibits a great potential application for high-performance HCDI systems.