Hydrogen transport by moving dislocations is one of the key mechanisms for hydrogen embrittlement, which is considered responsible for local hydrogen accumulation at preferential crack initiation sites. Although numerous experiments corroborate this mechanism, there are few theoretical models for it available. In the present work, a novel hydrogen transport model is developed within the coupled framework of crystal plasticity and hydrogen balance. The hydrogen transport flux in the present model is divided into two parts: the first-order hydrogen transport flux driven by plastic strain and the second-order hydrogen transport flux driven by plastic strain gradient. With the calibrated parameters by fitting experimental results, the first-order hydrogen transport flux is negligible even for nickel with a low hydrogen diffusivity. In polycrystals, due to the intrinsic plastic heterogeneity induced by grain orientation mismatch, the second-order hydrogen transport flux results in significant dynamic hydrogen segregation at grain boundaries during deformation, which is expected to drive the hydrogen-induced intergranular cracking as observed in experiments. This dynamic segregation behavior is related to the evolution rate of geometrically necessary dislocations, depending on the grain boundary characters. The roles of grain refinement in hydrogen transport are clarified with the present model. This study shows the vital role of plastic strain gradient induced by grain boundary constraint in hydrogen transport, which is essential in understanding hydrogen migration and accumulation in deformed polycrystalline metals.