Layered bulk crystals are amenable to exfoliation to yield 2D nanosheets through isolation and intercalation processes, which could be further converted to 1D nanoscale structures. The latter inherit gross morphological and physical properties associated with the precursor structures. Herein, we report three purine‐based crystal structures 1, 2, and 3, where 3 is obtained by a single‐crystal‐to‐single‐crystal transformation from 2 and is a conformational polymorph of 1. Next, we describe the sonication‐assisted liquid exfoliation of 1, a CdII–purine coordination framework, into nanosheets and nanofibers in a solvent‐dependent process. The exfoliation was carefully studied at low temperatures to ascertain this unique conversion. This work also features the determination of the Young's modulus and surface potential of the bioinspired CdII‐based nanostructures by using amplitude modulation–frequency modulation atomic force microscopy and Kelvin probe force microscopy, respectively, revealing their interesting elastic and capacitive properties for their possible use in electronics and energy devices. Electron impedance spectroscopy measurements further established a higher value of capacitance for the exfoliated CdII framework as compared to the ligand alone.