Developing efficient and affordable catalysts toward electrochemical reduction of CO2 to valuable chemicals is of great significance for energy and environmental sustainability, which can be efficaciously achieved by catalyst structure steering. In this study, we propose an ingenious strategy to modulate MoS2 favorable for CO2 reduction by fabricating an integrated three-dimensional (3D) TiO2@MoS2 architecture containing Ti-S bonds, the formation of which, revealed by density functional theory calculations, has changed the electric properties o...