Carbonaceous material is not only the excellent adsorbent for organic contaminants removal, but also the effective activator for peroxydisulfate (PDS) activation. In this study, a nitrogen-doped hierarchical porous carbon material (NHGBC-800) presented the attractive bifunctional properties was developed for the removal of model organic contaminant antibiotic tetracycline (TC). On the one aspect, the NHGBC-800 had a large specific surface area (1178.0 m2/g) and achieved good TC removal with a maximal adsorption capacity (Qm) of 629.76 mg/g at 303 K. On the other aspect, TC-saturated NHGBC-800 could effectively activate PDS with itself as the activator, by which the mineralization of desorbed TC and in-situ regeneration of exhausted adsorbent were achieved simultaneously. The Qm of NHGBC-800 recovered 90.61% after first regeneration and still retained 77.18% even after the 6th adsorption-regeneration cycles. Moreover, the as-prepared material maintained good adsorption and regeneration performance under a wide range of pH conditions (3.02–9.83) and in the presence of inorganic anions such as Cl−, SO42−, NO3−, H2PO4−, HCO3−. The electro spin resonance (ESR), reactive oxygen species (ROS) quenching studies and electrochemical measurement revealed that the electron-transfer and single oxygen mediated the non-radical pathways dominated the TC degradation during the regeneration process. Compared with the conventional thermal and electrochemical regenerations, the in-situ regeneration of bifunctional carbon materials induced by PDS activation is more effective, sustainable and environmental-friendly.