Shape-controlled synthesis of bimetallic nanocrystals has been one of attractive research directions in the fields of synthetic chemistry and catalysis. The driving force for the development of synthetic chemistry derives from the dependent relationship of the size, composition, shape and structure of nanocrystals with their catalytic performances. This chapter summarizes some significant achievements in preparing bimetallic nanopolyhedrons and nanospheres, and highlights shape effect of bimetallic nanocrystals on the associated catalytic performances. It is expected to provide some general ideas on the designed synthesis of shape-tunable bimetallic nanocatalysts with high performances.