A multiphase nanostructured ZrCu-base bulk alloy which showed a unique microstructure consisting of sub-micrometer scale Zr2Cu solid solution, nano-sized twinned plate-like ZrCu martensite (ZrCu (M)), and retained ZrCu (B2) austenite was fabricated by copper mold casting. The observation of periodic morphology evolution on the fracture surface of the multiphase nanostructured ZrCu-base alloys has been reported, which suggested a fluctuant local stress intensity along the crack propagation. It is necessary to investigate the compressive deformation behavior and the fracture mechanism of the multiphase alloy and the relation to the unique microstructures. The results obtained in this study provide a better understanding of the deformation and fracture mechanisms of multiphase hybrid nanostructured ZrCu-based alloys and give guidance on how to improve the ductility/toughness of bulk ZrCu-based alloys.