Process evaluation and optimization of the calcium looping system for the production of hydrogen from coal has been conducted using the commercial ASPEN Plus® process simulation software. The over all efficiency of this process for the production of 99.999% pure hydrogen from coal is 63% (HHV) when compared to the state-of-the-art, hydrogen from coal process which has an efficiency of 57% (HHV). The purity of hydrogen is increased by a large extent when the carbonation reaction is integrated with the WGSR. The steam addition for the WGSR can also be reduced to near-stoichiometric quantities which aids in reducing the parasitic energy consumption of the process. In addition, the extent of H2S removal by the CaO sorbent is also enhanced by operating at lower steam concentrations. High purity hydrogen of 99.7% with less that 1 ppm sulfur impurity has been obtained in a bench scale fixed bed reactor system. Experiments conducted in a bench scale system have revealed the superior performance of the OSU patented PCC based calcium oxide sorbent for the production of hydrogen.