One-step hydroxylation of benzene to phenol by N2O has been performed over structured catalytic beds made of ZSM-5 coatings on stainless steel grids. The catalysts demonstrated high activity with a selectivity toward phenol formation of 98%. A detailed kinetic study was carried out with a variation in reactant concentrations, benzene/N2O ratio, and residence time. The results obtained suggest a surface reaction between benzene and nitrous oxide adsorbed on two different active sites.