Previous attempts to establish global mass balances for polychlorinated dioxins and furans (PCDD/Fs) have focused on the terrestrial sink, thereby neglecting deposition to the oceans and atmospheric losses. In this study, the atmospheric sink of polychlorinated dioxins and furans (PCDD/Fs) was calculated on the basis of their presence in soils. OH radical ([OH]) depletion reactions compete with atmospheric deposition fluxes for the fate of atmospheric PCDD/Fs. Three different steady state scenarios were considered: scenario A was a one-box atmosphere with globally averaged [OH], temperature (T), atmospheric lifetime (tlife), and a constant gas-particle partitioning (Φ); in scenario B, [OH], T, and Φ were averaged in a multibox atmosphere, with a constant tlife; and in scenario C, tlife was varied. In scenario A the strength of the atmospheric sink was 2400–2800 kg/yr; in scenario B it was ∼2100 kg/yr; in scenario C, it was ∼1,800 kg/yr (tlife = 5.4 days) to ∼2,800 kg/yr (tlife = 14 days). The majority of the atmospheric sink was due to the depletion of Cl4DFs (1300–1400 kg/yr), followed by Cl4DDs (360–380 kg/yr) and Cl5DFs (230–240 kg/yr). On a global scale, major sinks for PCDD/Fs are the deposition to terrestrial soils and the oceans. For Cl6–8DDs, deposition to soils outweighs depletion reactions in the atmosphere and ocean uptake. The more volatile Cl4–5DD/Fs, however, are true “multimedia” compounds, with their estimated atmospheric sink being roughly as important as the terrestrial sink (in the case of Cl5DD/Fs) or outweighing it (e.g., Cl4DD/Fs).