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Three-dimensional Pd nanospheres have been fabricated by electrochemical deposition of Pd onto an indium tin oxide (ITO) glass substrate modified with a nanofibril film of poly(5-cyanoindole) (PCI).The size of Pd nanospheres could be controlled via simply adjusting the electro-deposition time.The morphology and structure of the Pd nanospheres were characterized by SEM,X-ray diffraction and electrochemical methods.The experimental results demonstrated that Pd nanospheres grew around the PCI nanowires and were fixed well on the PCI nanowires.The electrocatalytic activity of this electrode modified with three-dimensional Pd nanospheres was evaluated using formic acid as model molecules.The modified electrode showed improved electrocatalytic activity toward formic acid oxidation with respect to two-dimensional Pd nanoparticles directly deposited on ITO.