Liquid-phase mass-transfer coefficients are determined for the absorption of sulfur dioxide by wafer drops larger than 1.1 mm in dia. A local model based on the large eddy interfacial model proposed by Fortescue and Pearson (1967) is obtained by the characteristic interfacial scaling. In particular, the agitation process of the liquid phase in the interfacial region is characterized by the interfacial liquid friction velocity. Experiments of sulfur dioxide absorption and desorption from large individually free-falling water drops are also carried out in a 5-m rain shaft under various environmental conditions. These experimental results agree well with those from the local model characterizing the interfacial process in water drops greater than 1.1 mm in dia.