An efficient heterogeneous photocatalytic system for high-purity hydrogen evolution from formate or aldehyde-water solution were developed using IrCp*Cl (Cp* = eta(5)-pentamethylcyclopentadienyl) complex anchored onto the robust bipyridine-based organosilica nanotubes as a solid catalyst. This system can be conducted at the room temperature with a visible light (lambda > 420 nm) illumination. The heterogeneous molecular photocatalyst displayed much improved catalytic activity and recyclability compared to the analogous homogeneous catalyst, benefiting from the isolated photoactive sites as well as the efficient transport of substrates and products in the nanotube channels. A detailed characterization for the solid catalyst after the reactions by UV/vis, XPS and C-13 CP MAS NMR testified the molecular nature of the active species. This work provides an easy method to construct the heterogeneous molecular photocatalysts for the high-purity hydrogen generation under mild conditions.