A detailed investigation on the production of chlorine-free benzaldehyde in the solvent-free oxidation of benzyl alcohol by O₂ over nano-gold supported on U₃O₈ has been carried out. Influence of different catalyst parameters (different methods of gold deposition on U₃O₈, gold loading and particle size, and catalyst calcination temperature) and reaction conditions (reaction period and temperature) on the process performance has been studied. The catalyst containing gold at higher concentration and with smaller gold particles showed the better process performance (higher benzyl alcohol conversion and benzaldehyde yield or selectivity). The benzyl alcohol conversion is largely increased but the selectivity for benzaldehyde is slightly decreased (while that of benzyl benzoate is increased) with increasing the reaction period or temperature. In the presence of solvent (viz. tolune, p-xylene, DMF or DMSO), the process performance was found to be inferior to that observed in the absence of any solvent. Substituted benzyl alcohols also can be oxidized by O₂ to corresponding aldehydes with high yield and/or selectivity, using the catalyst in the absence of any solvent.