The lithium-carbon-hydrogen (Li-C-H) system is composed of hydrogenated nanostructural graphite (C(nano)Hx) and lithium hydride (LiH). C(nano)Hx is synthesized by ball-milling of graphite under a hydrogen atmosphere. In this work, the reaction process of hydrogen absorption and desorption on the Li-C-H system is investigated. The C(nano)Hx-LiH composite can desorb about 5.0 mass% of hydrogen at 350 degrees C with the formation of Li2C2 until the second cycle. However, the hydrogen desorption amount significantly decreases from the third cycle. Furthermore, it is shown by using gas chromatography that a considerable amount of hydrocarbons is desorbed during the rehydrogenation process. These results indicate that the amount of reaction between the polarized C-H groups in C(nano)Hx and LiH is reduced due to a decrease in the C-H groups by losing carbon atoms under the hydrogen absorption and desorption cycles.