Exploiting solar power for hydrogen production from seawater is a great challenge owing to the corrosive properties of seawater and inadequate visible-light conversion capabilities. Here we report an uncomplicated post-processing method to construct Ti3+ self-doped titanium-silicon material with corrosion resistance. This is a new experimental method to regulate the electrical, optical, and photocatalytic performances of titanium-containing photocatalysts in a controlled way. Moreover, we demonstrate that Ti-O-Si materials with different calcination temperatures can serve as a highly efficient and convenient catalyst for photogeneration of hydrogen from water and simulated seawater. Consequently, the optimized Ti-O-Si (400) sample exhibits impressive enhancement in the photocatalytic hydrogen evolution performance, by nearly 10.0 and 43.1 times compared with TiO2 nanoparticles in water and simulated seawater. The Ti-O-Si (400) with substantial Ti3+ and oxygen vacancies exhibits an excellent photocatalytic H2 production performance due to the improved separation and transmission of the photogenerated electron-hole, the extended visible light response, and corrosion resistance. Our work opens a new door to engineering the intrinsic properties of the titanium-containing materials.