Iron oxide pillars, less than 1 nm in height, were constructed in the interlayer of tetratitanate by the hydrothermal reaction of H2Ti4O9 and FeSO4 aqueous solution, followed by calcining in air. The samples showed absorption in the visible region and were capable of hydrogen evolution under visible light irradiation (lambda > 400 nm) in the presence of 0.1 M Na2S aqueous solution as a hole acceptor, although no noticeable hydrogen evolution was observed when H2Ti4O9 and Fe2O3 were used independently. Hydrogen evolution activity of iron oxide pillared tetratitanate increased by calcining in air at 300 degreesC after hydrothermal reaction.