Bimetallic nanomaterials are of great significance to both fundamental research and industrial applications.Their physicochemical performances are critically dependent on their architectures and electronic structures.Here,it was reported a controlled synthesis of Au/Ni bimetallic nanocrystals with different nanostructures,i.e.,dumbbell,core@shell and alloyed nanostructures in a onepot synthesis procedure.Detailed structural characterizations were conducted with the combination of transmission electron microscopy (TEM) and X-ray diffraction (XRD).Even there is a large lattice mismatch between Au and Ni,Au@Ni core@shell nanocrystals are obtained with the seeded growth method.The growth mechanism was deeply investigated.Triphenylphosphine is demonstrated to be an effective capping agent to modify the interfacial energy to form core@shell nanocrystals,and the higher temperature is proved to be a key role in obtaining alloyed nanocrystals.