A new system for the production of hydrogen, with a novel Maya blue-like organic-inorganic hybrid material as a photocatalyst, in which palygorskite acts as a matrix and Eosin Y as a photosensitizer, and Pt as a cocatalyst, has been reported. The pH value of the solution and the concentration of Eosin Y have remarkable effects on the rate of hydrogen evolution. It was also found that palygorskite has a significant effect on the rate of photosensitized hydrogen evolution. Electron transfer in photosensitized processes could be carried out via the dimers of Eosin Y. Based on the activities of hydrogen generation and the experimental measurements of UV-Vis absorbance and fluorescence, the probable mechanism for photosensitized hydrogen evolution has been postulated.