Several methods for evaluating separation quality in two-dimensional thin layer chromatography are discussed. These include using either the distance between spot centers for the pair of solutes that is the most difficult to separate in a mixture, or the value of a suitable separation function, as criteria of overall separation quality. Contour diagrams may be constructed in which solvent compositions for each of the two-dimensional developments are the independent variables and spot separation or the value of a suitable function is the dependent variable. Such diagrams indicate which are the best and the worst regions of the two-dimensional solvent domain. These diagrams should be of value for comparing different solvent systems for two-dimensional thin layer chromatography.