Samples of fresh penguin excrements and lake sediments composed of aged penguin excrements were collected on an Antarctic Peninsula island. Gases emitted from these samples were collected and analyzed for volatile organosulfur compounds. No dimethyl sulfide (DMS) was found. However, dimethyl trisulfide (DMTS), dimethyl tetrasulfide (DMTTS), and dimethyl pentasulfide (DMPS) were found among the numerous organic compounds emitted from fresh penguin droppings. These sulfur compounds account for as mush as 13.5% of the emitted gases, but they have not been reported previously in atmospheric gases and therefore may represent a hitherto undetected source of atmospheric sulfur. To evaluate the potential contribution of this non-DMS biogenic source to the atmospheric sulfur reservoir at high southern latitudes, measurements of various chemical species in aerosols at several coastal Antarctic locations were analyzed and compared. The locations include Zhongshan Station (China) and Dumont D'Urville (France) in east Antarctica. Tentative calculations based on assumptions of similar aerosol sources and composition at these locations show that in areas downwind from large penguin colonies up to 5.5 ¿ 10-5 nmol m-3 sulfur may be attributed to penguin emissions on a per-penguin basis. Depending on the size of penguin population at a given location, sulfur from this non-DMS source may account for 5--15% of the total non-sea-salt (nss) sulfur in these areas. Such high contributions may significantly impact the atmospheric sulfur burden and alter the sulfur budget in the high southern latitudes.