This study investigates harmony in two-colour combinations in order to develop a quantitative model. A total of 1431 colour pairs were used as stimuli in a psychophysical experiment for the visual assessment of harmony. These colour pairs were generated using 54 colours selected systematically front CIELAB colour space. During the experiment, observers were presented with colour pairs displayed individually against a medium gray background on a cathode ray tube monitor in a darkened room. Colour harmony was assessed for each colour pair using a 10-category scale ranging from "extremely harmonious" to "extremely disharmonious." The experimental results showed a general pattern of two-colour harmony, from which a quantitative model was developed and principles for creating harmony were derived. This model was tested using an independent psychophysical data set and the results showed satisfactory performance for model prediction. The study also discusses critical issues including the definition of colour harmony, the relationship between harmony and pleasantness, and the relationship between harmony and order in colour. (C) 2006 Wiley Periodicals, Inc.