Deuterium diffusion coefficient measurements of CVD-SiC were carried out using a solubility and diffusivity measurement apparatus to investigate the permeation mechanism of the hydrogen isotope through CVD-SiC. Experiments were conducted with thin-sheet-type samples with thicknesses of 0.1mm, 1mm, and 2mm at 1073–1183K. Total amount of occluded gas into or released gas from different thickness but same weight sample were expected to be the same, but unexpectedly differed by more than 50%. As the release rates after sufficient time had passed were almost the same, and the 1-mm-thick sample had twice the surface area of the 2-mm-thick sample, the measurements were probably affected by adsorbed gas on the surface. The value of D/L2 (the diffusion coefficient divided by the square of the thickness), obtained by fitting to the theoretical formula but ignoring the early phase of discharge, was in good agreement for samples of different thickness at the same temperature, and was more than 5 orders of magnitude smaller than that obtained from the permeability measurement experiments. Therefore, we believe that the deuterium permeation through CVD-SiC is primarily dependent on the permeation rate through the grain boundaries.