Sterilization methods and apparatus are effective to achieve a 6-log reduction in CFUs of industry standard bacteria and bacterial spores, i.e., B. stearothermophilus and B. subtilis spores, by subjecting sterilizable materials to a chemical additive-containing carbon dioxide sterilant fluid at or near its supercritical pressure and temperature conditions. Most preferably, the chemical additive-containing supercritical carbon dioxide sterilant fluid is agitated during sterilization, e.g., via mechanical agitation or via pressure cycling.