Photo-decomposition experiments to produce hydrogen from organic compound such as alcohols and organic acids were investigated using the Korean natural ilmenite, which was used as ore itself as well as the calcined in vacuum. The decomposition activities of alcohol on ore (30-60 mesh) which was not calcined did not decrease even if it was repeatedly used. But crushed ore which had newly formed ilmenite surface revealed enhanced activities. The ilmenite powder calcined in vacuum showed 3-8 times higher activies than the ore powder itself and also the decomposition activity of formic acid was much higher than that of alcohols.