Organic functional crystals with novel π-electronic states such as (super)conductivity, (anti-/ferro)magnetism, etc. have been vigorously developed. On the other hand, researches of hydrogen-related functionalities such as (anti-/ferro)electrics, proton (super)conductivity, etc. have been also extensively performed. In this article, the novel π-electron-hydrogen concerted organic materials and their functionalities are introduced. This phenomenon with dynamically coupled π electron-hydrogen might be related to biochemical cascade reactions and applicable to novel organic surface and devices.