AbstractGaseous elemental mercury (GEM) and 222Rn, a radioactive gas of primarily terrestrial origin with a half-life of 3.8 days, have been measured simultaneously at Cape Point, South Africa, since March 2007. Between March 2007 and December 2009 altogether 59 events with high 222Rn concentrations were identified. GEM correlated with 222Rn in 41 of the events and was constant during the remaining events without significant correlation. The average GEM/222Rn emission ratio of all events was −0.0047 ± 0.0054 pg mBq−1, with ± 0.0054 being the standard error of the average. With an emission rate of 1.1 222Rn atoms cm−2 s−1 and a correction for the transport duration, this emission ratio corresponds to a radon calibrated flux of about −0.53 ± 0.62 ng m−2 h−1 which is statistically not distinguishable from zero. With wet deposition, which is not included in this estimate, the terrestrial surface of southern Africa appears to be a net mercury sink.