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A series of material tests were performed on cryogenic metallic materials meant for liquid hydrogen storage tanks using a 20 K tensile cryostat and an electrochemical hydrogen-charging apparatus. Mechanical evaluation of the electrochemically hydrogen-charged specimens was performed in a tensile cryostat using helium gas at ambient temperature and cryogenic temperature (20 K). The tensile cryostat was equipped with a vacuum jacket and a G-M cryocooler with gaseous helium. Furthermore, the cathodic electrolysis cell used for charging the specimens was adopted for internal hydrogen conditions with a reflux condenser and heating mantle to increase hydrogen diffusivity. The target materials were austenite stainless steel and aluminum alloy, which are suitable for liquefied natural gas and gaseous hydrogen environments. No significant change in the yield strength and flow stress of the hydrogen-charged specimen up to 20% strain was observed. However, changes in tensile strength and elongation were observed thereafter. Electrochemical hydrogen charging of stainless steel leads to a high concentration of hydrogen on the surface of the specimen. The resulting surface cracks reduced the flow stress. The 20 K tensile test showed discontinuous yielding in the austenitic stainless steel with an abrupt increase in temperature. The mechanical performance of the aluminum alloys improved in terms of strength and elongation. Changes in the mechanical performance and relative area reduction were observed for all the metallic materials at 300 K and 20 K.