Probing the

Chirality plays a fundamental role in numerous scientific fields, yet the electronic structures of chiral compounds, particularly pairs of enantiomers, remain understudied. In this study, we address this gap by investigating the electronic structure of a chiral pair through single-crystal nuclear magnetic resonance (NMR) spectroscopy, complemented by X-ray diffraction and density functional theory (DFT) calculations. The combination of these techniques allows for the precise determination of the electronic environments of chiral molecules, offering direct insights into the subtle differences between enantiomers. Our results demonstrate the robustness of the capacity for experiment and computation to combine in resolving the NMR interaction tensors of enantiomers. This study advances our understanding of the chiral electronic structures of high-spin nuclei and the effects of chirality in various scientific contexts, although the potential for single-crystal NMR in stereochemical analysis remains a challenge for high-spin nuclei in asymmetric environments.