In this work we study the hydrogen generation by catalytic hydrolysis of alkaline NaBH4 solution employing Pd-supported on carbon powder (Pd/C) as well as in form of Pd and Pd-C thin films synthesized by pulsed laser deposition (PLD). Two sets of samples were prepared: (1) pure Pd catalyst films which were bombarded with Ar+ ions at different ions fluence in order to increase the surface roughness; (2) highly irregular C film were deposited by using different Ar pressure in the PLD chamber prior to deposition of the Pd film to further increase the surface area for the active I'd catalyst. Surface morphology was studied by using scanning electron microscopy (SEM) and atomic force microscopy (AFM) while compositional analysis was performed by using energy dispersive spectroscopy (EDS). Cone like structure on the surface of the Pd film developed by Ar+ ion bombardment was not efficient to enhance the catalytic activity of the Pd. Pd/C films showed higher catalytic activity in comparison to Pd/C powders when the same amount of catalyst is used. The results are discussed in relation to the morphology of the C-films. (C) 2007 International Association for Hydrogen Energy.