Effects of steam sterilization, gamma-irradiation, UV-irradiation and ozonation on microbial inactivation, pyrrolizidine alkaloid degradation and volatile compound profile in oregano were investigated. Steam sterilization and gamma-irradiation were the most effective treatments in inactivating microorganisms. These treatments resulted in 0.87–2.15 log reductions in total aerobic mesophilic bacteria counts and reduced yeast-mold and Enterobacteriaceae counts below the detectable level. Steam sterilization caused increased levels of pyrrolizidine alkaloids (PAs) and decreased levels of their N-oxide forms (PANOs) demonstrating a simultaneous conversion of PANOs into the corresponding PAs. Ozone treatment caused significant decreases in the levels of individual and total PAs/PANOs. After ozone treatment, decreases of 54.4, 53.9, 61.6 and 61.4% were observed in the levels of europine-N-oxide, europine, lasiocarpine-N-oxide and lasiocarpine, respectively. Steam sterilization, UV-irradiation and ozone treatments significantly altered the composition of the volatile compounds of oregano as evidenced by decreased levels of major components and the formation of some new compounds.