Development of alternative energy technologies is the key to address future energy concerns of depleting fossil fuel reserves and the hydrogen economy is one of the forerunners amongst the various options being considered. A combined hydrogen production and storage process was recently developed in which hydrogen was trapped within a coal-based structure, chemically modified via reactive ball milling. Low-temperature hydrogen evolution via Thermogravimetric analysis with mass spectroscopy (TG-MS), coupled with unusual Raman spectra, suggested both trapped molecular hydrogen and low-temperature dehydrogenation. Here we present the results of an investigation of the precursor coal structure in the resulting hydrogen evolution profiles. Our hypothesis is that ball milling induces carbon-cross links, further facilitated by solvent addition, and the cross-links correlate to trapped hydrogen. Several candidate anthracite coals were selected based on their amenability to form cross-links, using X-ray diffraction and temperature programmed oxidation to assess the graphitizability of the coal precursor. The relationship between hydrogen evolution, Multiwavelength Raman, and the graphitizability of the carbon precursor will be discussed.