Halogens influence the oxidizing capacity of Earth’s troposphere, and iodine oxides form ultrafine aerosols, which may have an impact on climate. We report year-round measurements of boundary layer iodine oxide and bromine oxide at the near-coastal site of Halley Station, Antarctica. Surprisingly, both species are present throughout the sunlit period and exhibit similar seasonal cycles and concentrations. The springtime peak of iodine oxide ( 20 parts per trillion) is the highest concentration recorded anywhere in the atmosphere. These levels of halogens cause substantial ozone depletion, as well as the rapid oxidation of dimethyl sulfide and mercury in the Antarctic boundary layer.