Considering the excessive emission of atmospheric carbon dioxide (CO₂) caused by the combustion of fossil fuels, the sunlight-driven CO₂ reduction into higher energy chemicals, such as carbon monoxide, formic acid, methanol or methane, offers a more promising approach to alleviate both global warming and energy crisis. Designing new photocatalytic materials for improving the photoconversion efficiency is a promising route to achieve this goal. Despite the invention of a large number of catalytic materials with well-defined structures, their overall efficiency in photocatalysis is still quite limited as the three key steps - light harvesting, charge generation and separation, and charge transfer to surface for redox reactions - have not been substantially improved. To improve each step in the complex process, there is a major trend to develop materials based on inorganic hybrid structures, in which surface and interface engineering holds the promise for boosting the overall efficiency. In this talk, I will demonstrate several different approaches to designing inorganic hybrid structures with improved photocatalytic performance via surface and interface engineering. It is anticipated that this series of works open a new window to rationally designing inorganic hybrid materials for photo-induced applications.