Li-C-H system, which can store about 5.0 mass% of rechargeable H 2 , has been reported as a promising hydrogen storage system by Ichikawa et al. [Appl. Phys. Lett. 86, 241914 (2005); Mater. Trans. 46, 1757Trans. 46, (2005]. This system was investigated from the thermodynamic and structural viewpoints. However, hydrogen absorption/desorption mechanism and the state of hydrogen atoms absorbed in the composite have not been clarified yet. In order to find new or better hydrogen storage system, graphite powder and nano-structural graphite ball-milled under H 2 and Ar atmosphere were prepared and milled with Li and Mg under Ar atmosphere in this study. Microstructural analysis for those samples by transmission electron microscope revealed that LiC 6 and/or LiC 12 were formed in Li-C-H system. On the other hand, MgC 2 was found in Mg-C-H system ball-milled under H 2 atmosphere, but not in the system ball-milled under Ar atmosphere. These results indicated that nano-structure in composites of nano-structural graphite is different from that of alkali (-earth) metal. For these reasons, metal-C-H system can be recognized to be a new family of hydrogen storage materials. V C 2013 AIP Publishing LLC.