For electrochemical hydrogen evolution reaction (HER), developing high-performance catalysts without containing precious metals have been a major research focus in the present. Herein, we show the feasibility of HER catalytic enhancement in Ni-based materials based on topological engineering from hybrid Weyl states. Via a high-throughput computational screening from ∼140,000 materials, we identify that a chiral compound NiSi is a hybrid Weyl semimetal (WSM) showing bulk type-I and type-II Weyl nodes and long surface Fermi arcs near the Fermi level. Sufficient evidences verify that topological charge carriers participate in the HER process, and make the certain surface of NiSi highly active with the Gibbs free energy nearly zero (0.07 eV), which is even lower than Pt and locates on the top of the volcano plots. This work opens up a new routine to develop no-precious-metal-containing HER catalysts via topological engineering, rather than traditional defect engineering, doping engineering, or strain engineering.