Titanosilcalite-1 (TS-1)-supported gold catalysts (Au/TS-1) are promising for propene oxide (PO) synthesis through gas-phase propene epoxidation with hydrogen and oxygen. Herein, we report an efficient and simple approach to promote the catalytic activity of Au/TS-1 using dual-component promoters, namely, Na and Cs. The prepared catalyst exhibited a much better activity compared with the general catalyst using a single alkali metal promoter. Further characterization results of NH3-TPD-MS, C3H6-TPD-MS, HAADF-STEM, and Si-29 MAS NMR show that the enhancement of activity is highly associated with the modified surfaces of TS-1 by the dual-component Na-Cs promoters and the optimized gold loading. Meanwhile, the role of anions such as CO32- in this catalytic system could not be neglected.