It is important to investigate the mechanical performances of (Gd0.9Yb0.1)2Zr2O7 (GYbZ)materials deposited on irregular substrates for improving new thermal barrier coatings. Three-point bending fracture characteristics of freestanding GYbZ coating prepared by supersonic plasma sprayed (SPS) technique were investigated with the help of digital image correlation technique. The cracking time, crack propagation path, and mechanical properties of GYbZ coating were obtained. Meanwhile, the X-ray computed tomography technique was introduced to scan the microstructure of freestanding GYbZ coatings, which are used to establish three-dimensional (3D) finite element model by using the Avizo software. The brittle cracking criterion was applied to describe the bending fracture process of GYbZ coatings. The critical cracking strain was estimated as 0.36％±0.03％ by repeatedly comparing the difference between the experimental and simulated curves. The results would be extended to predict the dangerous region and failure mechanisms of GYbZ coatings deposited on irregular substrate during finite element simulations.