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A moderately concentrated solution of a helically chiral polyisonitrile forms a stable two‐phase system in CDCl3 with the dense phase being close to isotropic and the less dense layer forming a completely anisotropic lyotropic liquid crystalline phase. This enables the enantiodifferentiating measurement of isotropic and anisotropic NMR parameters from a single sample by novel spatially resolved NMR methods. More information can be found in the Full Paper by M. Reggelin, B. Luy et al. on page 13351. [ABSTRACT FROM AUTHOR]