To investigate hydrogen embrittlement susceptibility of an individual grain boundary, microcantilevers were fabricated on Ni-Cr bialloy surfaces by focused ion beam, and microbending tests were conducted during hydrogen charging by electrochemical nanoindentation. For microcantilevers fabricated across a twin boundary and inside a grain, no crack was formed by the bending both in air and during hydrogen charging. On the other hand, for microcantilevers fabricated across a random grain boundary, a crack was formed by the bending during hydrogen charging, whereas no crack was formed in air. Thus, it was identified that, for Ni-Cr bialloy, random grain boundaries are more susceptible to hydrogen than twin boundaries and crystalline planes. To validate these experimental results, slow strain-rate tensile tests were also performed, and subcracks of the fractured specimens were analyzed by electron beam back-scattering diffraction. In accordance with the microbending test results, subcracks were predominantly formed along random grain boundaries, but never along twin boundaries and inside grains. Higher hydrogen susceptibility of the random grain boundaries with lower cohesive energy (i.e., work for separation), smooth fracture surfaces without dimples or tear ridges, and no correlation between strain accumulation and subcrack formation indicate that hydrogen embrittlement of Ni-Cr bialloy is caused by decohesion mechanism, where hydrogen atoms lower cohesive energy at grain boundaries.