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PM3 SCF calculations have been carried out to study the thermolyses of o-acetylcycolpentanone and o-acetylcyclohexanone. The results obtained show that these two com-pounds are thermally decomiposed into products through an unimolecular elimination involving six-center cyclic transition state, and these two thermolyses are caused by the migration of posi-tive charged β-H.