A ZIF-derived Co, N-doped graphitic carbon prepared by calcination exhibited excellent carbamazepine (CBZ) removal ability over a broad pH range for peroxymonosulfate (PMS) activation. The impact of calcining temperature on catalyst constitution and catalytic behavior were studied through characterization and performance experiments. Benefiting from the synergy of adsorption and catalysis, CZIF-1000/PMS (with a 1000 °C pyrolysis temperature) system demonstrated outstanding catalytic capability, with 96.8 % removal efficiency supported by optimum parameters (catalyst dosage, 50 mg/L, PMS dosage, 0.4 mM, CBZ concentration, 5 ppm, and initial pH, 5.8). The graphitic N, pyrrolic N, CO group, Co3+ and Co0 were revealed to be the activation centers by X-ray photoelectron spectroscopy (XPS). Mechanisms exploration suggested that dual active pathways, including singlet oxygen-dominated non-radical pathway and sulfate radical-dominated radical pathway were involved in the reaction mechanism. Besides, a total of ten intermediates were detected and CBZ degradation pathways were derived subsequently.