A rapid, templateless, surfactantless, electrochemical route is reported to synthesize uniform and clean Pd nanoparticles (∼350 nm in diameter) with a substructure of sharp nanospikes (∼95 nm in length). The effects of electrodeposition potential, PdCl(2) concentration, and supporting electrolyte were explored for the formation of the Pd nanourchins. The systematic studies revealed that the concentration of Pd(II) greatly affects the density of the nanospikes on the Pd nanourchins in this short-time synthesis. The substructure of the nanospikes on the nanourchins was examined to be a single-crystal quadrangular pyramid. Further investigation of the Pd nanourchins by cyclic voltammetry (CV) showed their high electrochemical activity toward formic acid oxidation.