Abstract: In-situ failure analysis of metallic structural materials plays a key role in understanding the fracture mechanism and improving the performance of components. Synchrotron Radiation X-Ray Computed Tomography (SR-μCT) has advantages of high spatial and high temporal resolution, and thus are widely used in the research on the failure behavior of metallic structural materials. The applications of SR-μCT in the aluminum matrix and layered composites and the recent research on the failure behavior were summarized. The advanced characterization techniques were also introduced. Combining SR-μCT with Diffraction Contrast Tomograph, the grain orientation and grain boundary characters can be obtained. Combining SR-μCT with Digital Volume Correlation, the in-situ 3D strain field can be obtained. Building the correlations among 3D structure, orientation, composition, strain field, and developing in-situ failure analysis method will become research hot spots.