Gas transport parameters and X-ray computed tomography (CT) measurements in porous medium under controlled and identical conditions provide a useful methodology for studying the relationships among them, ultimately leading to a better understanding of subsurface gaseous transport and other soil physical processes. The objective of this study was to characterize the relationships between gas transport parameters and soil-pore geometry revealed by X-ray CT. Sands of different shapes with a mean particle diameter (d50) ranging from 0.19 to 1.51 mm were used as porous media under both air-dried and partially saturated conditions. Gas transport parameters including gas dispersivity (α), diffusivity (DP/D0), and permeability (ka) were measured using a unified measurement system (UMS). The 3DMA-Rock computational package was used for analysis of three-dimensional CT data. A strong linear relationship was found between α and tortuosity calculated from gas transport parameters (Equation (Uncited) Image Tools), indicating that gas dispersivity has a linear and inverse relationship with gas diffusivity. A linear relationship was also found between ka and d50/TUMS2, indicating a strong dependency of ka on mean particle size and direct correlation with gas diffusivity. Tortuosity (TMFX) and equivalent pore diameter (deq.MFX) analyzed from microfocus X-ray CT increased linearly with increasing d50 for both Granusil and Accusand and further showing no effect of particle shape. The TUMS values showed reasonably good agreement with TMFX values. The ka showed a strong relationship when plotted against deq.MFX/TMFX2, indicating its strong dependency on pore size distribution and tortuosity of pore space.