A chemical heat pump system using two hydrogen-absorbing alloys is proposed to utilise heat exhausted from a high-temperature source such as a high-temperature gas-cooled reactor (HTGR), more efficiently. The heat pump system is designed to produce H2 based on the S-I cycle more efficiently. The overall system proposed here consists of HTGR, He gas turbines, chemical heat pumps and reaction vessels corresponding to the three-step decomposition reactions comprised in the S-I process. A fundamental research is experimentally performed on heat generation in a single bed packed with a hydrogen-absorbing alloy that may work at the H2 production temperature. The hydrogen-absorbing alloy of Zr(V1-XFeX)2 is selected as a material that has a proper plateau pressure for the heat pump system operated between the input and output temperatures of HTGR and reaction vessels of the S-I cycle. Temperature jump due to heat generated when the alloy absorbs H2 proves that the alloy–H2 system can heat up the exhaust gas even at 600°C without any external mechanical force.