Bowl-like nanostructures of Pt/Pd bimetallic nanocrystals are prepared by employing Ag nanoparticles as a template and completely removing the residual Ag after the displacement. Scanning electron microscopy (SEM) and transmission electron microscopy (TEM) observations display that the thin walls of Pt/Pd nanobowls are composed of nanoparticles. X-ray diffraction (XRD) pattern demonstrates that Pt and Pd form the alloy in the nanobowls. The crystal structures of the nanobowls consist of [111], [200], [220] surfaces as revealed by both high-resolution TEM (HRTEM) and XRD results. The Pt/Pd nanobowls exhibit significant high electrocatalytic activities toward the methanol oxidation and oxygen reduction compared with the Pt/Pd nanospheres and Pt nanobowls.