An effective way to improve the catalytic activity of metal-based nanostructured materials is to control the size, shape, or composition. Here, the bimetallic PdPt nanoparticles (NPs) show significant dependency on the shape for catalytic hydrolysis of ammonia borane. The catalytic activity of PdPt cubic nanoparticles (cNPs) is found to be the best compared with the activities of spherical nanoparticles (sNPs) of Pd, Pt, and PdPt and cNPs of Pd under the same reaction conditions. The turnover frequency (50.02 min(-1)) of PdPt cNPs for ammonia borane hydrolysis is among the values of the most active catalysts. This high catalytic performance of PdPt cNPsencourages the approach of shape and composition control for various catalytic applications.