Formerly, S. Yamatodani and M. Abe obtained lysergol as well as two new basic compounds, lysergene and lysergine, by chemical experiments. These compounds had not been found in nature, but lately S. Yamatodani demonstrated by paper chromatography the existence of three unknown substances ("a", "b" and "c") considered to be lysergol, lysergene and lysergine in the sclerotia and saprophytic cultures of some ergot fungi. Recently, we have succeeded in isolating "a", "b" and "c" in crystalline form from the saprophytic cultures of ergot fungi—the former two from the surface culture of Elymus-type ergot fungus and the latter from the culture of a strain belonging to the Agropyron-type fungus—either by counter current distribution or column chromatography using Hyflo Super Cell treated with a McIlvaine buffer solution. Substance "a" was identical with lysergol, "b" with lysergene, and "c" with lysergine based on their physical and chemical properties (melting point, optical rotation, elemental analysis, color reactions, UV and IR spectra). The present results support our previous presumption that the same path shown in previous chemical conversion experiments exists in nature.