Chiral surfaces are critical components of enantioselective heterogeneous processes such as those used to prepare enantiomerically pure pharmaceuticals. While the majority of chiral surfaces in practical use are based on achiral materials whose surfaces have been modified with enantiomerically pure chiral adsorbates, there are many inorganic materials with valuable surface properties that could be rendered enantiospecific, if their surfaces were intrinsically chiral. This Perspective discusses recent developments in the fabrication of intrinsically chiral surfaces exhibiting enantiospecific adsorption, surface chemistry and electron emission. We propose possible paths to the scalable fabrication of high-surface-area, enantiomerically pure surfaces and discuss opportunities for future progress.