AbstractSupported gold catalysts play a crucial role in the chemical industry; however, their poor on-stream stability because of the sintering of the gold nanoparticles restricts their practical application. The strong metal-support interaction (SMSI), an important concept in heterogeneous catalysis, may be applied to construct the structure of catalysts and, hence, improve their reactivity and stability. Here we report an ultrastable Au nanocatalyst after calcination at 800 °C, in which Au nanoparticles are encapsulated by a permeable TiO_x thin layer induced by melamine under oxidative atmosphere. Owning to the formed TiO_x overlayer, the resulting Au catalyst is resistant to sintering and exhibits excellent activity and stability for catalytic CO oxidation. Furthermore, this special strategy can be extended to colloidal Au nanoparticles supported on TiO₂ and commercial gold catalyst denoted as RR2Ti, providing a universal way to engineer and develop highly stable supported Au catalysts with tunable activity.