<p>Topological catalysts are special class of high-activity catalysts that have topological surface state with high-mobility electrons to promote electron transfer. Among topological materials, high-fold degenerate topological semimetals (TSMs) with chiral structures are particularly effective in hydrogen evolution reaction (HER) catalysis due to the larger energy window of nontrivial surface states and longer Fermi arcs than other classes. In this work, based on high-throughput calculations and the database of high-fold degenerate TSMs with chiral structures that we have established, we predict 16 high-activity topological catalysts with Gibbs free energy ∣ΔG∣ smaller than that of Pt. Among them, PtGa and PtPbTe with space group P2₁3 and Pd₃Pb₂S₂ with space group I2₁3 exhibit outstanding catalytic behavior. Furthermore, by comparing the adsorption energy on the surfaces with and without topological surface state in the same compound straightly, the substantive fact that the extremely long topological surface state provides virtual improvement of HER catalytic performance is verified. Thus, this work not only discovers a lot of HER topological catalysts, but also provides and corroborates an innovative strategy to design high-activity catalysts, i.e., constructing monometallic catalysts into TSMs.</p>