It is well known that the terminal velocity of a drop settling in a viscous fluid is impacted by surface tension gradients. These gradients can develop because of nonuniform accumulation of surfactant on the surface as a result of a number of transport mechanisms. Here, a surfactant transport model based on a sorption-limited Frumkin framework is used to describe surfactant transport in the presence of both surface convection and diffusion at low Reynolds and capillary numbers. Constants characterizing surfactant transport in the Frumkin framework are experimentally determined and used to predict aqueous drop velocities with varying surfactant concentrations and volumes. Computation is carried out by satisfying equations governing mass, momentum, and interface species conservation. Experiments demonstrate qualitative and quantitative agreement between predicted and measured drop velocities. It is shown that surface remobilization explains some observed trends in measured velocity as the drop size decreases. (c) 2018 American Institute of Chemical Engineers AIChE J, 65: 294-304, 2019