The effect of irregular polygonal grain size and random grain boundary on hydrogen diffusion in polycrystalline nickel is investigated. Hydrogen diffusion behavior in micropolycrystalline nickel is compared with that in nanopolycrystalline nickel through numerical analysis. The two dimensional computational finite element microstructural and nanostructural analyses are based on Fick's law corresponding to heterogeneous polycrystalline model geometry. The heterogeneous polycrystalline model consists of random irregular polygonal grains. These grains are divided into internal grain and grain boundary regions, the size of which is determined from the grain size. The computational analysis results show that hydrogen diffusion in nanostructural irregular polycrystalline nickel is higher in magnitude than the microstructural irregular polycrystalline nickel. However, models of voids, traps and micro and nano clustered grains are yet to be included.