The temperature-dependent fracture toughness of WC-10Co4Cr coating/1018 low carbon steel substrate, which is a brittle coating/ductile substrate system, is evaluated at microscopic level with two types of models developed in terms of the Arrhenius-type equation and rate controlling theory, utilizing indentation test data, in this research. One is based on the crystal structures of individual phases in the composite coating, the other considers the microcrack formation in the coating/substrate system under indentation loading. Using the crystal-structure-based model, the slip systems of the hard hexagonal -WC phase and soft FCC -Co phase are analyzed. The fracture toughness of the two-phase composite coating is obtained by integrating the fracture toughness of -WC phase and -Co phase using either the basic mixture method or the unconstrained mixture method. The estimated fracture toughness using this type of model is independent of indentation load. For the microcrack-formation-based models, numerous microcracks are generated from each corner of indentation impression and merge together to form radial cracks due to the tension of residual stresses in the coating/substrate system under indentation, and the radial cracks extend along the indentation diagonals under the residual stresses. The dislocation movement of atoms can be associated with the microcrack formation in the indentation process thus the fracture toughness of the composite coating/substrate system is evaluated. Due to the effect of ductile substrate on brittle coating, two approaches are used to investigate the indentation pressure imposed on the system, one expresses the indentation pressure as the applied load ii divided by the projected area of indentation impression, the other is based on the composite hardness of the coating/substrate system, but both approaches take the substrate effect into the fracture toughness evaluation. The estimated fracture toughness of WC-10Co4Cr coating/1018 low carbon steel substrate system at high temperatures shows that the crystal-structure-based model and microcrack-formation-based models are in good agreement. The fracture toughness of WC-10Co4Cr coating/1018 low carbon steel substrate system remains unchanged until the temperature reaches a critical value, 200 for crystal-structure-based model, 150 for microcrack-formation-based models. It then increases rapidly in an exponential manner. The room-temperature fracture toughness of the coating/substrate system obtained from all models is about 2.1 ⁄ , the fracture toughness at 1000 ranges from 8.5669 ⁄ to 11.2399 ⁄ using different models and under different indentation loads. iii Acknowledgements I owe my sincere gratitude to my supervisors, Professor Rong Liu, for her constant support and guidance during my research and study at Carleton University. Her expert knowledge and endless patience are invaluable and indispensible for me to finish this thesis.