Unusual Surface Texture, Dimensions and Morphology Variations of Chiral and Single Crystals**

We demonstrate here a unique metallo‐organic material where the appearance and the internal crystal structure are in contradiction. The egg‐shaped (ovoid) crystals have a brain‐like texture. Although these micro‐sized crystals are monodispersed; like fingerprints their grainy surfaces are never exactly alike. Remarkably, our X‐ray and electron diffraction studies unexpectedly revealed that these structures are single‐crystals comprising a continuous coordination network of two differently shaped homochiral channels. By using the same building blocks under different reaction conditions, a rare series of crystals have been obtained that are uniquely rounded in their shape. In stark contrast to the brain‐like crystals, these isostructural and monodispersed crystals have a comparatively smooth appearance. The sizes of these crystals vary by several orders of magnitude.
The egg‐shaped homochiral crystals: A brain‐like texture combined with single crystallinity. A series of isomorphous crystals found in a rare space group have been formed with varied morphologies. These crystals contain chiral channels and are made from achiral components.