A study was made of mass transfer rates from single large oscillating drops of pure liquidliquid systems, in the size range of 5 to 10 mm. A thermostatically-controlled, 50 mm in diameter, 1000 mm long, rising drop column was used, in which mirrors in the jacket enabled front and side views of drops to be photographed simultaneously. The systems studied were 1) toluene and acetone (dispersed)-water (continuous), and 2) n-heptane and acetone (dispersed)-water (continuous). High concentrations of acetone (up to 3.75 kmol/m3) were used to examine the effect of different parameters on the mass transfer rate, frequency and amplitude of oscillation in countercurrent operation. Previous theories and empirical correlations [2-6, 12, 13, 151 for the prediction of overall mass transfer coefficients showed large deviations from measured values. These may have arisen because the models do not represent droplet oscillation accurately, and/or apply only to oscillations of small droplets. Fair agreement was obtained for small oscillating droplets at low solute concentrations. The oscillations of a travelling drop were asymmetrical; the period of oscillation was uniform for mutually-saturated systems but changed when mass transfer was taking place. The periods were longer than those predicted by the Lamb [7] and Shroeder and Kintner This will facilitate more accurate prediction of the dispersed phase mass transfer coefficients relating to equipment containing droplets in the oscillating regime, e.g. pulsed columns or agitated tanks.