<p>High-fold degenerate topological semimetals (TSMs) that can host fermions with high-fold degeneracy have attracted considerable interest recently, but not many topological materials have been verified. Among them, ones with chiral structure possessing larger topological charge and extremely long Fermi arcs bring about some special properties like topological catalysis. Here, based on high-throughput calculations and density functional theory, we have built a program to search high-fold degenerate fermions automatically. A database including 146 chiral high-fold degenerate TSMs with exotic fermions near the Fermi level is established and described in detail. It contains not only the well-known CoSi family of materials, but also a sight of new TSMs originating from 14 space groups. The high-fold degenerate points in chiral structures are three-, four-, or sixfold and exist at the high symmetry k-points. Moreover, these TSMs containing high-fold degenerate fermions can also host Weyl points in chiral structures, which can also be valuable for the achievement of quantum Hall effect, quantized circular photogalvanic effect, and so on.</p>