Following the success in understanding the textures in TiSi2 (C49) epitaxy on (001)(Si) surface using the edge-to-edge matching model that was originally developed for predicting the crystallographic features of diffusion-controlled phase transformations in solids, the present work applies this model to understand the in-plane texture in TiSi2 (C54) thin films on Si single crystal surfaces and to explain why its epitaxial growth is more favoured on (111)(Si) than on (001)(Si). Based on the actual atomic spacing along the matching directions across the interface between the thin films and the substrate, the model predicts most of the experimentally observed orientation relationships (ORs) and that the preferred order among the different systems is C49/(001)(Si) system>C54/(111)(Si) system> C49/(111)(Si) system congruent to C54/(001)(Si) system. The model has strong potential to be used to develop new thin film materials. (c) 2007 Elsevier B.V. All rights reserved.