Drying-induced birefringence of polyimide film was investigated. The polyimide solutions were coated and dried on two different types of substrates and then removed for optical measurements. The operating window, which was a region for stable and uniform film formation, was determined experimentally. The out-of-plane birefringence (OPBR) was found to increase with decreasing dry film thickness, and the increase became more significant for films less than 10 mu m thick. The experimental OPBR results were compared with the predictions of two theoretical models. The results agreed reasonably well with the one-dimensional model of Lei et al. (J Appl Polym Sci. 2001;81:1000-1013). On the other hand, a simple viscoelastic model, which is an extension of the elastic model of Croll (J Appl Polym Sci. 1979;23:847-858), could provide clear physical insight, but its applicability was somewhat limited. The effects of several variables such as elasticity number, solidification concentration, yield stress, and mass transfer rate on OPBR were examined. (C) 2009 American Institute of Chemical Engineers AIChE J, 56: 790-800, 2010