An analysis of the solidification rates of binary mixture melts flowing as a thin film on a cold surface, useful in the separation or purification of eutectic mixtures, is presented. The analysis which incorporates the hydrodynamics of the falling film and the convective heat transfer at the melt/crystal interface was used to determine the average crystallization velocity. The effect of parameters such as Stefan number (subcooling), initial superheat and the melt loading rate on the average crystallization velocity was examined. Experiments were performed using three different binary organic mixtures at subeutectic compositions. The results of the theoretical and experimental studies showed good agreement validating the model. © 1999 OPA (Overseas Publishers Association) N.V.