The synthesis of atomically dispersed metal clusters with strong interaction with the support is attractive for the design of high-efficiency catalysts. Here, we report a multilayered catalyst (1.91%Pt@TiO 2 ), in which atomically dispersed Pt clusters are encapsulated in the porous TiO 2 . As a result, 1.91%Pt@TiO 2 exhibited high activity, selectivity (92.9%), and excellent stability in the semi-hydrogenation of phenylacetylene.