Qualitative and quantitative understanding of Po volatilization under different conditions is of key importance for safety assessments of lead-bismuth eutectic (LBE) based nuclear reactors, spallation targets and accelerator driven systems. In this work we explore the possibilities of the transpiration method in combination with simple models to study the equilibriumand kinetics of Po evaporation fromhighly diluted solutions in lead-bismuth eutectic between 600 and 1000 ∘Cin Ar/5%H 2 andAr. On the basis of evaporation experiments at various carrier gas flow rates, we identified the conditions of vapor saturation allowing the determination of equilibrium constants. Fromthe limiting behavior athigh flowrates, values for the maximal evaporation rate of Po from LBE were estimated. Measurements of evaporation as a function of time were consistent with the assumption that poloniumdissolved in LBE obeys Henry’s law. A theoretical analysis furthermore suggested that diffusion of polonium in LBE was not a rate limiting factor for evaporation under vapor saturation conditions. Newly determined values for theHenry constant of Po in LBE between 600 and 1000 ∘C were consistent with previously derived correlations.