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A tooth-whitening process using hydrogen peroxide (H2O2) enhanced by a direct-current cold atmospheric-pressure plasma microjet (PMJ) is presented. Compared with the conventional clinical method of using H2O2 alone, a significant improvement of the tooth-whitening process was observed when the PMJ was used in the process. The tooth-surface temperature was monitored for safety considerations and did not exceed 37°C at a distance of 1 cm between the exit nozzle of the plasma source and the tooth for a treatment time of 20 min. No apparent differences in the tooth-surface morphology and microhardness were observed between teeth treated with and without the PMJ. The use of the PMJ with H2O2 resulted in an enhanced production of reactive hydroxyl (OH) radicals. This plasma-enhanced tooth-whitening method may be a promising new method for clinical applications.