A vanadium pentoxide supported activated coke (V 2 O 5 /AC) catalyst-sorbent has been reported to be very active for simultaneous removal of SO 2 and NO under dry conditions at temperatures of 200°C and below. Regeneration of the SO 2 -captured catalyst-sorbent is a key step in operation of such a process, which influences the catalyst-sorbent's SO 2 and NO removal activities, lifetime, as well as recovery of sulfur. Due to limited information in this regard, this paper studies thermal regeneration of a V 2 O 5 /AC catalyst-sorbent with emphases on the effect of atmosphere. The optimum regeneration temperature is found to be 380°C in an Ar stream and 300°C in a 5% NH 3 /Ar stream. Compared to the fresh V 2 O 5 /AC, the V 2 O 5 /ACs regenerated in Ar show lower SO 2 adsorption capacities and higher NO removal activities, while the regenerated V 2 O 5 /ACs by 5% NH 3 /Ar show higher and stable SO 2 adsorption capacities and higher NO removal activities. Two types of reactions occur during the regeneration: reduction of the adsorbed sulfur species by carbon to SO 2 and CO 2 , and oxidation of carbon by oxygen in the V 2 O 5 /AC to CO 2 . The carbon consumption of the latter is much more than that of the former in an Ar atmosphere, but fully suppressed by the presence of 5% NH 3 . Detailed analysis and characterization of the V 2 O 5 /AC subjected to the regenerations are presented.