A sample containing Pd nanoparticles deposited on TiO2 was subjected to a series of different thermal pretreatments. The range of these treatments was selected to provide a palladium surface in a number of different states, including a form where TiOx overlayers had been formed. Experiments were conducted to determine how the state of the Pd surface influenced the formation of Pd hydride. The amount of hydrogen released during a temperature-programmed experiment was used to quantify the extent of Pd beta-hydride formation following room-temperature exposure to hydrogen. Samples were characterized by HAADF (high-angle annular dark-field) electron microscopy with EDX (energy-dispersive X-ray) analysis and CO pulse chemisorption and FTIR (Fourier transform infrared spectroscopy) of adsorbed CO. The amount and the ease with which Pd beta-hydride was formed was found to be dependent on the metal surface area, the presence of titania overlayers, and the Pd surface roughness/defect concentration.