Although chiral purity is a critical quality attribute for many synthetic drugs, current industrial strategies for establishing chiral purity control are underdeveloped. Such strategies have relied on the construction of ternary phase diagrams, system classification, and case-specific operating policies. These policies have been developed to provide enantiopure solids, regardless of product specification or target. In this article, new operating policies are developed for obtaining solids that meet, but do not exceed, chiral purity specifications for arbitrary systems. These policies can provide significant yield improvements over the current practice. Additionally, this work provides an approach for the creation of design spaces based on the collection of limited, small scale data. This approach has been extended to sequential re-crystallizations and can be used to determine global optimal policies within a synthetic route. (c) 2018 American Institute of Chemical Engineers AIChE J, 64: 3323-3331, 2018