The evaluation of activities from radionuclides inside a vacuum vessel is required for the safe maintenance and estimation of the activation level of fusion devices. The Large Helical Device (LHD), Toki, Japan, has been performing deuterium plasma experiments since 2017, and radionuclides have accumulated in components such as vacuum vessels. In this work, the gamma-ray spectrum and activity of each detected radionuclide in an LHD vacuum vessel were evaluated using portable high-purity germanium (P-HPGe) and numerical calculations of photon transport for comparison with the removed armor tiles to evaluate the occupational exposure in the maintenance of LHD experiments. Measurements using the P-HPGe detector were performed at 20 positions along the toroidal direction of the LHD, at each O port, and between each pair of adjacent O ports. Using the estimated efficiency of the photoelectronic effects inside the P-HPGe detector calculated by Monte Carlo N-particle code version 6.1, the activities of the radionuclides in the armor tiles attached to the vacuum vessel were evaluated. The estimated activity concentrations were compared with the measured activities of the armor tiles removed from the vacuum vessel. Gamma rays from 58Co, 54Mn, and 60Co were detected, and the measured activities of 58Co and 54Mn generated by fast neutrons in the armor tile were almost consistent with those obtained from the removed armor tiles. The radioactivity of 60Co in the armor tile was underestimated compared with the activity obtained from the removed armor tiles. The measurement of activation by fast neutrons is feasible, whereas activation by thermal neutrons requires more accurate calculations and surveys to be measured using this method.