The effect of hydrogen on the deformation and fracture behavior in pure Cu, pure Ni and Cu-Ni alloy was studied via tensile tests of H-charged, smooth and circumferentially-notched specimens at room temperature (RT) and 77 K. Hydrogendiffusion properties were determined by the desorption method. To obtain a uniform hydrogen concentration in the H-charged specimens, specimens were exposed to 100-MPa hydrogen gas at 543 K for 200 h, based on the determined hydrogen diffusivity. In tensile tests of smooth pure Ni and Cu-Ni alloy specimens at RT, common hydrogen effects were detected, namely, an increase in yield and flow stresses-a hardening effect; and a ductility loss that was accompanied by a change in fracture surface from ductile to brittle feature-an embrittling effect. With regard to the embrittling effect, the pure Ni and Cu-Ni alloy showed different fracture-surface morphologies at RT; the pure Ni showed an intergranular (IG) surface and the Cu-Ni alloy surface was flat. However, a number of IG cracks were detected beneath the fracture surfaces on the smooth Cu-Ni alloy. The tensile tests of the H-charged smooth specimens at 77 K yielded an IG surface for the pure Ni and a ductile fracture surface with dimples in the Cu-Ni alloy. In contrast, tensile tests of the Hcharged, notched specimens at RT demonstrated clear IG fractures for the pure Ni and Cu-Ni alloy. These facts indicate that IG cracking was the first step in the embrittling process for the pure Ni and Cu-Ni alloy, and IG cracking was accompanied by a large plastic deformation that formed the flat surface (unclear IG surface) for the smooth Cu-Ni alloy. Considering that the HE of both pure Ni and Cu-Ni alloy was related to IG cracking, possible mechanisms were discussed and tensile tests performed at 77 K suggested two possibilities: (I) interaction between hydrogen-moving dislocation is more important in the HE process of the Cu-Ni alloy compared to the pure Ni; (II) hydrogen transportation towards grain boundaries are required to cause the IG fracture in the Cu-Ni alloy.