In order to meet the demand of metal hydride–hydrogen compressors (MHHC) and their hydrogen compression materials for high-pressure hydrogen filling in a hydrogen energy field, four kinds of hydrogen storage alloys with low-grade heat source (<373 K) heating outputs and different hydrogen pressures (up to 80 MPa) were developed as hydrogen compression materials. The preliminary compositions of the hydrogen storage alloys were determined by using a statistical model and research experience. The rare earth series AB₅ and Ti/Zr base AB₂ hydrogen storage alloys were prepared using a high-temperature melting method. The composition, structure, and hydrogenation/dehydrogenation plateau characteristics of the alloys were tested by an inductively coupled plasma mass spectrometer (ICP-MAS), X-ray diffractometer (XRD), and pressure–composition isothermal (PCT) tester. The median output pressures of the four-stage hydrogen storage alloys at 363 K were 8.90 MPa, 25.04 MPa, 42.97 MPa, and 84.73 MPa, respectively, which met the requirements of the 20 MPa, 35 MPa, and 70 MPa high-pressure hydrogen injections for the MHHCs. In fact, due to the tilted pressure plateau of the PCT curve, the synergy between the adjacent two alloys still needed to be adjusted.