For the purpose of developing an effective system for hydrogen isotope separation, we have been studying the adsorption-desorption dynamic behavior of hydrogen and deuterium in a packed-bed column with synthetic zeolites, aimed at applying the pressure swing adsorption process. The adsorption behavior of molecules in the packed-bed is reflected in the breakthrough curves. To understand the characteristic behaviors of hydrogen isotopes in the packed-bed, we carried out breakthrough experiments in a conventional adsorption process and in a practical process following sequential processes alternating between adsorption and desorption. From the former experiments, the results were obtained that the overall mass transfer was influenced by longitudinal dispersion relating to the superficial velocity and that the process governing the mass transfer within adsorbents was diffusion in the macro-pores of pellets. In the latter experiments, unique profile breakthrough curves were observed. These curves can be described with the numerical simulation assuming the initial distributions in a packed-bed.