The application of peptide and peptidomimetic chiral selectors in LC is reviewed in this article. In particular, methods for finding these types of selectors using combinatorial library approaches are discussed, as well as recent advances in the use of peptides and peptidomimetics as general chiral selectors for LC. In terms of the library approaches, batch screening and reciprocal screening are discussed. As for general chiral selectors, one example involves the application of chiral diamide phases. Another example shows the versatility of oligoproline chiral stationary phases, which exhibit resolution for a number of racemic analytes, comparable to other well-established chiral stationary phases.