This report presents an accelerated kinetic Monte Carlo (KMC) method to compute the diffusivity of hydrogen in hcp metals and alloys, considering both thermally activated hopping and quantum tunneling. The acceleration is achieved by replacing regular KMC jumps in trapping energy basins formed by neighboring tetrahedral interstitial sites, with analytical solutions for basin exiting time and probability. Parameterized by density functional theory (DFT) calculations, the accelerated KMC method is shown to be capable of efficiently calculating hydrogen diffusivity in α-Zr and Zircaloy, without altering the kinetics of long-range diffusion. Above room temperature, hydrogen diffusion in α-Zr and Zircaloy is dominated by thermal hopping, with negligible contribution from quantum tunneling. The diffusivity predicted by this DFT + KMC approach agrees well with that from previous independent experiments and theories, without using any data fitting. The diffusivity along is found to be slightly higher than that along , with the anisotropy saturated at about 1.20 at high temperatures, resolving contradictory results in previous experiments. Demonstrated using hydrogen diffusion in α-Zr, the same method can be extended for on-lattice diffusion in hcp metals, or systems with similar trapping basins.The diffusion of hydrogen in hcp metals has attracted extensive research interests for both its scientific merit and technological importance. It is the rate-limiting step for solid hydrogen storage in Mg based alloys 1 and for mechanical property degradation in Ti 2 and Zr alloys 3 . For instance, Zr-based alloys such as Zircaloy2 and Zircaloy4 (denoted as Zircaloy) are widely used as the cladding of fuel rods in nuclear reactors for their excellent corrosion resistance and very low absorption cross-section of thermal neutrons. During their service time, these alloys operate in extremely harsh environments, combining high temperatures and corrosive coolants such as water. In light water reactors, Zircaloy claddings directly contact coolant water, with a local temperature at the interface of about 400 °C. Consequently, Zircaloy react with water, producing an oxide layer at the interface and hydrogen (H), of which a substantial fraction infiltrates into the cladding interior 3 . Due to the low solubility of H in α -Zr, which is the main component of claddings, hydrides precipitate in the cladding matrix 4-6 . Hydride formation can detrimentally affect the cladding integrity primarily in two ways. First, the formation of hydrides reduces the fracture toughness of the cladding matrix 7,8 , increasing the probability of fuel failure when fuel-cladding mechanical interaction (PCMI) occurs during fuel operation. Second, upon cyclic thermal and mechanical loadings, hydrides can dissolve and reorient. During used-fuel storage, fracture may propagate via the so-called delayed-hydride-cracking (DHC) mechanism, which is induced by the dissolving of matrix hydrides and their subsequent re-formation at crack tips 3,9 . To mitigate thes...